Coherent Diffractive Imaging Near the Spatio-Temporal
Limit with High-Harmonic SourcesbyDennis Floyd Gardner Jr.
B.A., University of Colorado, 2010
M.S., University of Colorado, 2013

A thesis submitted to the
Faculty of the Graduate School of the
University of Colorado in partial fulfillmentof the requirements for the degree ofDoctor of Philosophy
Department of Physics
2017This thesis entitled:
Coherent Diffractive Imaging Near the Spatio-Temporal Limit with High-Harmonic Sources
written by Dennis Floyd Gardner Jr.
has been approved for the Department of Physics

Prof. Margaret M. Murnane

Prof. Henry C. Kapteyn

Date

The final copy of this thesis has been examined by the signatories, and we find that both thecontent and the form meet acceptable presentation standards of scholarly work in the above
mentioned discipline.

iii
Gardner Jr., Dennis Floyd (Ph.D., Physics)
Coherent Diffractive Imaging Near the Spatio-Temporal Limit with High-Harmonic Sources
Thesis directed by Prof. Margaret M. Murnane and Prof. Henry C. Kapteyn

This thesis discusses methods for high-resolution static and stroboscopic microscopy using
tabletop coherent extreme ultraviolet (EUV) radiation from tabletop high-harmonic generation(HHG) sources. These coherent short wavelength light sources are combined with a lensless,computational, phase and amplitude-contrast technique called ptychographic Coherent Diffractive
Imaging (CDI). While ptychographic CDI techniques are currently widespread for visible, EUV and
X-ray microscopy, no previous work has been able to achieve at-wavelength resolution of extended
samples, especially in a reflection geometry, nor has previous work been able to image periodic
samples with high-fidelity. In this work, a combination of experimental methods for high-numericalaperture imaging and novel computational algorithms enabled the highest resolution-to-wavelength
demonstrations using any CDI technique. These algorithms include tilted plane correction, whichenables high-resolution imaging of surfaces in a reflection geometry, and a powerful techniquetermed modulus enforced probe, which enables both imaging of periodic objects and convergenceof the ptychographic CDI algorithm in fewer iterations. Furthermore, the ultrafast pulse duration of the high-harmonic radiation is harnessed to demonstrate proof-of-principle pump-probe
imaging of nanostructures, capturing thermal transport processes in nanostructures with an axial
resolution of 3 angstroms. Stroboscopic imaging with nanoscale resolution is a critical tool for theinvestigation of nanoscale heat flow and magnetic switching for the advancement of next generation
nano-electronics, data storage, and nano-engineered systems.

Dedication

For my parents, Myriam and Dennis Gardner Sr.
For my partner, Corinne Beier.

v

Acknowledgements

I would like to express my gratitude to my research advisers, Professor Margaret Murnane
and Professor Henry Kapteyn, for their vision, leadership, and enthusiastic encouragement. I am
also grateful for Professor Daniel Adams whose guidance has shaped this work and my professional
development.
I wish to acknowledge the entire Kapteyn-Murnane imaging team whom I worked closelywith over the years and whose assistance impacted nearly every aspect of this work. Thank you
Elisabeth Shanblatt, Giulia Mancini, Christina Porter, Robert Karl Jr., Michael Tanksalvala, andCharles Bevis. I would also like to acknowledge my predecessors, Matt Seaberg and Bosheng Zhang,whose efforts are the foundation of this work.
I greatly appreciate the assistance provided by the thermal-acoustics team during the assembly and testing of the dynamic experiments. Thank you Jorge “Nico” Hernandez-Charpak, Travis
Frazer, and Josh Knobloch.
Thank you KM Labs, especially Xiaoshi Zhang, for both technical equipment and advice.
My special thanks to the JILA staff and shops: the electronics shop; the Keck Laboratory andDavid Alchenberger; and the instrument shop with Todd Asnicar, Hans Green, Kim Hagen, Blaine
Horner, Kyle Thatcher, and the late Tracy Keep.
And finally, I wish to acknowledge my undergraduate mentors, Professor Ivan Smalyukh
and Professor Noah Finkelstein, whose early support, encouragement, and advocacy were very
influential in my academic development.

Contents

Chapter
1 Introduction

1

2 A Tour of Microscopy

4

3 Coherent Sources of EUV and X-rays

9

3.1

3.2

Large Scale Facilities . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

9

3.1.1

Synchrotrons . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

9

3.1.2

X-ray Free-Electron Lasers . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11

Tabletop Sources . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
3.2.1

EUV Lasers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14

3.2.2

High-Harmonic Generation . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14

4 High-Harmonic Generation

16

4.1

Driving Laser . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16

4.2

HHG - The Microscopic Picture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18

4.3

HHG - The Macroscopic Picture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19

4.4

Temporal Characteristics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21

5 Imaging Forming Methods with EUV and X-rays

24

6 Coherent Diffractive Imaging

30

6.1

History of Phase Retrieval . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 30

vii
6.2

Oversampling and the Isolation Constraint . . . . . . . . . . . . . . . . . . . . . . . . 31

6.3

Ptychography . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34
6.3.1

History . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34

6.3.2

Ptychographic Data Collection . . . . . . . . . . . . . . . . . . . . . . . . . . 35

6.3.3

The Ptychography Algorithm . . . . . . . . . . . . . . . . . . . . . . . . . . . 37

7 Coherent Diffractive Imaging in a Reflection Geometry
7.1

7.2

41

Aperture-Illumination Coherent Diffractive Imaging . . . . . . . . . . . . . . . . . . 41
7.1.1

Transmission mode AICDI . . . . . . . . . . . . . . . . . . . . . . . . . . . . 42

7.1.2

Reflection mode AICDI . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 43

Near-Wavelength Resolution CDI in Reflection with EUV . . . . . . . . . . . . . . . 47
7.2.1

High numerical aperture data collection of scattered EUV . . . . . . . . . . . 47

7.2.2

Reconstructing high-NA reflection geometry data using CDI . . . . . . . . . . 49

7.2.3

Resolution Characterization . . . . . . . . . . . . . . . . . . . . . . . . . . . . 52

8 Sub-wavelength coherent imaging of a periodic sample

54

8.1

Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 54

8.2

Experimental set-up and Modulus Enforced Probe methodology . . . . . . . . . . . . 56

8.3

Intensity assignment to the extracted zero-order diffraction peak . . . . . . . . . . . 57

8.4

Sub-wavelength coherent imaging of extended near-periodic objects . . . . . . . . . . 61

8.5

Implementation of the Modulus Enforced Probe Constraint . . . . . . . . . . . . . . 67

8.6

Modulus Enforced Probe Simulations . . . . . . . . . . . . . . . . . . . . . . . . . . . 70

8.7

Conclusion. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 73

9 Stroboscopic Imaging of Thermal Transport in Nanostructures

75

9.1

Pump-Probe Principles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 76

9.2

Experimental Geometry . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 76

9.3

Experimental characterization of the Time-resolved ptychographic CDI microscope . 82

viii
9.4

Dynamics from a gold circuit-like sample . . . . . . . . . . . . . . . . . . . . . . . . . 85

9.5

Statistical significance of the phase shifts . . . . . . . . . . . . . . . . . . . . . . . . . 93

9.6

Calculation of the height change from thermal expansion . . . . . . . . . . . . . . . . 95

9.7

Summary and Future work . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 96

10 Conclusion

98

10.1 Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 98
10.2 Future Work . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 99
10.3 Future Outlook . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 100

104

Bibliography

Appendix
A From Maxwell to Fraunhofer

119

A.1 The Wave Equation from Maxwell’s Equations . . . . . . . . . . . . . . . . . . . . . 119
A.2 Diffraction by a Planar Screen. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 121

A.3 Huygens Principle . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 123
A.4 The Fresnel Approximation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 124
A.5 Fraunhofer Diffraction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 125
A.6 Angular Spectrum of Plane Waves . . . . . . . . . . . . . . . . . . . . . . . . . . . . 125
A.7 Propagation Applicability and the Fresnel Number . . . . . . . . . . . . . . . . . . . 128
B Tilted Plane Correction

129

B.1 Normal Incidence Geometry . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 129
B.2 Scattering with Normal Incidence Illumination . . . . . . . . . . . . . . . . . . . . . 131
B.3 Tilted Plane Correction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 132
C Near-Wavelength Resolution CDI in Reflection with EUV: supplemental figures

134

ix
D Sub-wavelength coherent imaging of periodic samples: supplemental figures

137

D.1 Full ptychographic reconstruction of the zone plate sample . . . . . . . . . . . . . . . 137
D.2 Phase images with and without the MEP constraint . . . . . . . . . . . . . . . . . . 138
D.3 Random Initial Probe Guess Simulations . . . . . . . . . . . . . . . . . . . . . . . . . 139
D.4 White Gaussian Noise Simulations . . . . . . . . . . . . . . . . . . . . . . . . . . . . 140

xTablesTable
8.1

Reconstruction parameters for the 13nm work . . . . . . . . . . . . . . . . . . . . . . 67

8.2

Modulus Enforced Probe Simulation Parameters . . . . . . . . . . . . . . . . . . . . 71

8.3

Fewer iterations to converge with MEP . . . . . . . . . . . . . . . . . . . . . . . . . . 73

9.1

Statistical significance determined with a t-test . . . . . . . . . . . . . . . . . . . . . 95

Figures

Figure2.1

Numerical Aperture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

5

2.2

Electromagnetic Spectrum . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

8

3.1

Radiation from Relativistic Electrons . . . . . . . . . . . . . . . . . . . . . . . . . . . 10

3.2

Free-Electron Laser . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13

4.1

Mode-locked laser cavity alignment . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17

4.2

Chirped Pulsed Amplification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18

4.3

High-Harmonic Generation - The Microscopic Perspective . . . . . . . . . . . . . . . 20

4.4High-Harmonic Generation - The Macroscopic Perspective . . . . . . . . . . . . . . . 22

5.1

Compound Refractive Lens . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25

5.2

Fourier Transform Holography

5.3

Various EUV and X-ray Optical Elements . . . . . . . . . . . . . . . . . . . . . . . . 29

6.1

CDI with Error-Reduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32

6.2

Oversampling and a Isolated Object . . . . . . . . . . . . . . . . . . . . . . . . . . . 33

6.3

Overlap and Probe Shifts . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38

6.4

Ptychography data collection and flowchart . . . . . . . . . . . . . . . . . . . . . . . 40

7.1

Aperture-Illumination Setup . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 44

7.2

Aperture-Illumination Transmission Imaging. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 27

. . . . . . . . . . . . . . . . . . . . . . 45

xii
7.3

Tilted Plane Correction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 46

7.4

Aperture-Illumination Reflection Imaging . . . . . . . . . . . . . . . . . . . . . . . . 48

7.5

High-NA reflection geometry and sample . . . . . . . . . . . . . . . . . . . . . . . . . 50

7.6

Tilted Plane Correction in the EUV . . . . . . . . . . . . . . . . . . . . . . . . . . . 51

7.7High-Resolution EUV imaging in a reflection geometry . . . . . . . . . . . . . . . . . 53

7.8

Three-Dimensional Rendering from the Phase Information . . . . . . . . . . . . . . . 53

8.1

Modulus enforced probe coherent EUV microscopy . . . . . . . . . . . . . . . . . . . 58

8.2

Modulus enforced probe methodology . . . . . . . . . . . . . . . . . . . . . . . . . . 60

8.3

Record sub-wavelength resolution imaging using 13.5 nm light and Modulus Enforced
Probe . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 63

8.4

Zone plate PMMA feature lineout and topographic image . . . . . . . . . . . . . . . 63

8.5

Minimization of cross-talk with the modulus enforced probe constraint . . . . . . . . 66

8.6

Modulus Enforced Probe implementation within ptychography algorithm

8.7

Ptychography with MEP: simulated sample . . . . . . . . . . . . . . . . . . . . . . . 72

8.8

Perfect Initial Probe Guess Simulated Reconstruction . . . . . . . . . . . . . . . . . 72

9.1

Pump-Probe Timing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 77

9.2

Pump-Probe Schematic . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 79

9.3

The pump-probe experimental chamber . . . . . . . . . . . . . . . . . . . . . . . . . 81

9.4

Verifying time zero with a grating sample . . . . . . . . . . . . . . . . . . . . . . . . 84

9.5

Static Gold Circuit Reconstruction . . . . . . . . . . . . . . . . . . . . . . . . . . . . 86

9.6

Dynamic Signal from Circuit Diffraction . . . . . . . . . . . . . . . . . . . . . . . . . 87

9.7

Negative Time Phase Distribution . . . . . . . . . . . . . . . . . . . . . . . . . . . . 90

9.8

Positive Time Phase Distribution . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 91

9.9

Statistical t-test on gold phase distributions . . . . . . . . . . . . . . . . . . . . . . . 94

10.1 EUV imaging through metal. . . . . . 69

. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 101

xiii
10.2 Possibilities for future work . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 103
A.1 Diffraction from Planar Screen from a Point Source . . . . . . . . . . . . . . . . . . . 122
A.2 Mirror Point Source . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 122
A.3 Diffraction Geometry in Cartesian Coordinates . . . . . . . . . . . . . . . . . . . . . 124
A.4 Angular Spectrum Propagation Between Two Planes . . . . . . . . . . . . . . . . . . 126
B.1 Coordinate Definitions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 130
B.2 Low NA with Normal Incidence . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 133
B.3 High NA with Normal Incidence . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 133
B.4 High NA with Non-Normal Incidence . . . . . . . . . . . . . . . . . . . . . . . . . . . 133
C.1 Full-Field, high-contrast, ptychographic imaging with high-harmonic generation . . . 134
C.2 Later Resolution Characterization . . . . . . . . . . . . . . . . . . . . . . . . . . . . 135
C.3 Axial Resolution Characterization . . . . . . . . . . . . . . . . . . . . . . . . . . . . 136
D.1 Full ptychographic image of the zone plate sample . . . . . . . . . . . . . . . . . . . 137
D.2 Phase images of the zone plate sample . . . . . . . . . . . . . . . . . . . . . . . . . . 138
D.3 Random Initial Probe Guess Simulation Results . . . . . . . . . . . . . . . . . . . . . 139
D.4 White Gaussian Noise Simulations . . . . . . . . . . . . . . . . . . . . . . . . . . . . 140

Chapter 1

Introduction

Understanding the structure and evolution of materials at greater spatial and temporal resolutions is central for discovery and innovation in science and technology, accelerating advances inmaterials and energy science, as well as nano-electronics and medicine. Many systems of interest
have features on the order of nanometers (10−9 s) with dynamics occurring at picosecond (10−12s) to femtosecond (10−15 s) time scales. For example, heat transport of closely packed nanoscale
structures or the ultrafast switching of magnetic materials; both have important technologically
impacts in current and next-generation nano-electronics devices and data storage systems.
A stroboscopic microscope using coherent extreme ultraviolet (EUV) radiation from highharmonic generation sources is an ideal tool to investigate ultrafast nanoscale phenomena, because
the short wavelengths allow nanoscale resolution and short pulses can capture the fastest dynamics.
Imaging with EUV has been challenging due to the lack of refractive-lenses and because most
EUV optics are costly, imperfect, lossy, and cannot reach diffraction-limited spatial resolution.
Fortunately, coherent diffractive imaging (CDI) has overcome this limitation by replacing image
forming optics with computation. In CDI, the diffracted light from the sample is recorded, andusing iterative phase retrieval algorithms, the diffracted light is back propagated to reconstruct
a complex-valued image of the sample. The resolution in CDI is not limited by optics, instead
it is only limited by the wavelength of illumination and the numerical aperture of the recorded
diffraction pattern.
While CDI techniques are widely used for visible, EUV, and X-ray microscopy, no previous

2
work has been able to achieve at-wavelength resolution of extended samples, especially in a reflection
geometry, nor has previous work been able to image periodic samples with high-fidelity. The
ability to image in a reflection geometry is important for investigation of nano-patterned structureson substrates, substrates too thick for transmission imaging, and the ability to image periodic
structures is especially important for industrial applications.
In this work, a combination of experimental methods for high-numerical aperture imaging
and novel computational algorithms, enabled the highest resolution-to-wavelength demonstrations
using any CDI technique in the EUV and x-ray spectral regions. These algorithms include tilted
plane correction, which enables high-resolution imaging of surfaces in a reflection geometry, and apowerful technique termed modulus enforced probe, which enables quantitative imaging of periodic
objects and convergence of the ptychographic algorithm in fewer iterations. In reflection, 40nm
resolution was obtained with 30nm EUV, and in transmission, 12.6 nm resolution was obtained ona quasi-periodic sample using the technologically relevant wavelength of 13.5 nm.
Furthermore, the ultrafast pulses from high-harmonic generation were harnessed in the construction of a novel stroboscopic EUV microscope. Proof-of-principle pump-probe imaging of nanostructures is demonstrated, capturing thermal transport processes in nanostructures with an axial
resolution of 3 angstroms.
This thesis is organized as follows. An overview of microscopy, with attention to nanoscaleand dynamic imaging capabilities, is given in Ch. 2. Due to their short wavelengths, sources ofextreme ultraviolet and x-rays are ideal for nanoscale imaging. The generation of EUV and x-rays
is the subject of Ch. 3 with emphasis on coherent sources capable of producing ultrafast pulses.
Following the overview on sources, Ch. 4 is devoted specifically to high-harmonic generation.
Given the lack of conventional refractive lenses, many techniques have been developed toimage in the EUV and x-ray spectral regions and is the topic of Ch. 5. Chapter 6, is dedicated tocoherent diffractive imaging, including ptychography.
The bulk of this thesis is contained in the following three chapters. In Ch. 7, methods,
including tilted-plane correction, are discussed for reflection geometry CDI. The powerful modulus

3
enforced probe methodology, which enables both imaging of periodic objects and faster convergenceof the ptychographic CDI algorithm, is presented in Ch. 8. And in Ch. 9, the ultrafast pulse
durations of the high-harmonic source were harnessed to demonstrate proof-of-principle pumpprobe imaging of nanostructures capturing thermal transport processes. This thesis concludes witha discussion of ongoing and future work in Ch. 10.

Chapter 2

A Tour of Microscopy

Since the first scientific publication using a microscope in 1665 by Robert Hooke [1], microscopy has led to many discoveries impacting just about every aspect of our lives.1

In 1873,

Ernst Abbe, developed a criteria for the fundamental resolution limit of a microscope,∆r =λ2n sin θ(2.1)

where ∆r is the resolution, λ is the wavelength of light, n is the refractive index, and θ is thehalf-angle of the light collected by the imaging lens (see Fig. 2.1). The term n sin θ is defined as
the numerical aperture, NA, of the imaging system, allowing the fundamental resolution limit tobe written as,
∆r =

λ
.
2 NA

(2.2)

In modern microscopes, oil is used between the sample and the imaging lens to increase the NA by
increasing the index of refraction n. Using oil immersion lenses the NA can be increased to values
around 1.4, leading to resolutions around 180 nm using visible wavelengths (500 nm).
Many strategies have been developed to beat the diffraction limit, such as multiphoton excitation, near-field imaging, and super-resolution techniques. Multiphoton techniques use two, or
more, IR photons to excite fluorescent molecules. Multiphoton microscopy can achieve higher resolution than the diffraction limit, around 100nm [4, 5], because only a localized spot within thefocus of the illumination reaches sufficient intensity for the excitation of the dye molecules. The
1

A review of visible microcopy is given in Ref. [2].

5Figure 2.1: Numerical Aperture The diffraction limited resolution of an imaging system isdependent the numerical aperture (NA). The lens, shown in blue, is characterized by its pupil
diameter, D, and its focal length f. Figure adapted from [3].

6
multiphoton approach, can also be applied without dyes, using a technique known as Coherent
anti-Stokes Raman scattering (CARS) [6], in which the multiple photons map the sample’s vibrational states. However, the improvements in resolution that multiphoton techniques achieved are
not sufficient to resolve nanoscale structures.
Another strategy, Nearfield Scanning Optical Microscopy (NSOM) [7, 8], theoretically discussed in 1928 [9], and then experimentally demonstrated in the microwave region with resolution
60× smaller than the illumination wavelength [10] in 1972. In NSOM, an aperture with a diametersmaller than the illuminating wavelength is brought near the sample and evanescent waves arerecorded near the sample. The limit on resolution in no longer dependent on the wavelength of illumination, but instead is dependent on the size of the aperture, and demonstrations have achieved
spatial resolution on the order of 10’s of nm using optical wavelengths [11]. Furthermore, pulsed
lasers have been applied to this technique for ultrafast temporal resolution on the order of 100’s of
femtoseconds [12].
The 2014 Noble prize in chemistry was awarded to pioneers of super-resolution techniques now
widely used in biology [2]. These methods use fluorophores and are commonly referred to by theiracronyms STED, PALM, and STORM. In Stimulated emission depletion (STED) microcopy, theemission area of the fluorescent spot is reduced by using doughnut beams created with diffractive
optical elements [13, 14]. The doughnut beams are tuned to suppress emission of the dyes except
for a nanometer sized volume at the center, which is stimulated with another laser.
Photoactivated localization microscopy (PALM) and stochastic optical reconstruction microscopy (STORM), use the stochastic blinking of the fluorophores [15, 16]. With sparse emitting
fluorophores, computation models can pinpoint the location of the emitters with nanometer precision [17]. While the resolution of STED, PALM, and STORM are impressive, on the order of 10
nm, they are not suitable for ultrafast dynamic investigations because the excitation and emissionof the dye molecules is on the order of nanoseconds, and is too slow to capture the picosecond to
femtosecond dynamics of many scientifically relevant systems.
Instead of super resolution techniques with optical wavelengths to achieve nanometer reso-

7
lution, another strategy is to decrease the wavelength of illumination. Due to the wave-particle
duality of nature, fast electrons can be described as waves given by de Broglie’s equation [18]
λ =

h
p

(2.3)

where λ is the wavelength, h is Plank’s constant, and p is the momentum. The momentum is mass
times velocity, with the velocity of electron’s typically described by its kinetic energy in electron
volts (eV). A modest energy for a modern electron source is 100keV, corresponding to an electron
wavelength of approximately 3 picometers (pm), orders of magnitude smaller the visible light waves.
Knoll and Ruska harnessed these short wavelengths and developed the first electron microscope in1931 [19].2 Theoretically, electron microscopes should have been able to obtain atomic resolution
from their inception, but atomic resolution was not demonstrated for decades due to aberrations
in electron lenses [22]. Currently, pulsed laser sources are being combined with electron sources
to create ultrafast electron microscopes [23, 24]. It is a promising technique, but still has many
challenges to overcome, such as space charge effects in the electron packets, which spread the pulse
widths to about 100 femtoseconds [25].
Half of the 1986 Nobel Prize in physics went to Ruska for the invention of the electron
microscope, the other half of the prize went to Rohrer and Binnig for point-scanning microscopy.
In point-scanning microscopy, the resolution is not dependent on wavelength, but instead on the
sharpness of a tip. The first demonstration is the scanning tunneling microscope in 1981 [26],followed by the atomic force microscope in 1986 [27]. In a scanning tunneling microscope, a charged
tip is brought very near the surface such that electrons tunnel from the surface into the tip enablingatomic sensitivity. The atomic force microscope (AFM), is not quite as sensitive, but it is commonlyused to profile nanoscale features with angstrom axial resolution [27]. In the AFM, a tip is mounted
on the end of a cantilever and the cantilever is raster-scanned across the sample. If there arechanges in sample height, the tip is attracted or repelled by atomic forces and deflections of thecantilevers are monitored to from a detailed profile of the surface. These point scanning methods
2

A history of electron microscopy is given in Refs. [20, 21].

8
are powerful nanoscale techniques, and have been combined with pulsed optical lasers for dynamic
experiments [28, 29].
Complementary to the techniques described previously, coherent extreme ultraviolet (EUV)and x-rays are well suited for nanoscale imaging because of their short wavelengths. The wavelengths of EUV range from 100 nm to 10 nm, and x-rays range from 10 nm to 0.01 nm (see Fig. 2.2).
As the Abbe resolution criterion scales with wavelength, Eq. 2.1, these sources are theoreticallycapable of achieving nanometer scale resolution, without any super resolution techniques. Furthermore, depending on the source, coherent EUV and x-rays are capable of capturing the fastest of
dynamics with pulses in the picosecond, femtosecond, or even attosecond regime [30]. The generation of coherent EUV and x-rays is the topic of the next chapter.

Figure 2.2: Electromagnetic Spectrum Most microscopes today employ wavelengths in thevisible region of the spectrum. The microscopes developed during this thesis use extreme ultraviolet
radiation, which lies between the ultraviolet and x-ray regions, for high resolution microscopy.
Figure adapted from [31].

Chapter 3

Coherent Sources of EUV and X-rays

Sources of coherent EUV and x-rays can be divided into two categories: large and small scale
sources. Large scale sources harness the radiation emitted by relativistic electrons and require alarge accelerator facility. Small scale sources, on the other hand, do not require particle accelerators,
drastically reducing their cost and size.

3.1

Large Scale Facilities
Large scale facilities can be further divided into synchrotrons and free-electron lasers (FEL).

In both facilities electrons are accelerated with radio waves to nearly the speed of light. Electrons
are used, instead of protons, because their lighter mass allows for greater speeds given the sameenergy input. As discussed below, the faster the electrons, the harder and brighter the source.

3.1.1

Synchrotrons

In a synchrotron, relativistic electrons are kept on a closed path using bending magnetics witha burst of radiation produced at each bending magnet. First generation synchrotrons operated
parasitically off pre-existing electron storage rings used for particle physics. Second generation
facilities were built as dedicated facilities for EUV and x-ray experiments with bending magnetics
all around the facility. These facilities were optimized to keep the electrons circulating for 5100 hours, allowing time for measurements [32]. Modern third generation synchrotrons employ
additional magnets, wigglers and undulators, to generate harder and brighter radiation. [33]

10Figure 3.1: Radiation from a Relativistic Electron a) Slow moving electrons produce dipolelike radiation patterns. b) In the laboratory frame, electrons traveling at relativistic speeds emit
radiation in a narrow, ‘searchlight’ type pattern. Figure adapted from Ref. [36].

When the velocity of a charged particle is small compared to the speed of light, the powerradiated per unit solid angle has the characteristic sin2 (θ) dependence given bydP
e2 2 2=a sin (θ),
dΩ
4πc3

(3.1)

where e is the electron charge, c is the speed of light, a is the acceleration, and θ is the angle
between the acceleration and the velocity. This dipole-like radiation is shown in Fig. 3.1a. Whenthe velocity of the electron approaches the speed-of-light, the radiation pattern is altered due torelativistic effects. The dipole-like radiation, Eq. 3.1, can be generalized for arbitrary velocities
using the appropriate Lorentz transformations [34]. When generalized and adapted for acceleration
perpendicular to the electron’s velocity the radiation distribution is given by,dP
e2
a2
sin2 (θ)cos2 (φ)
=
[
1
−
]
dΩ
4πc3 (1 − βcos(θ))3γ 2 (1 − βcos(θ))2
where β ≡ v/c and γ ≡

p

(3.2)

1 − β 2 [34, 35]. This radiation is sharply peaked in the forward direction

and the divergence angle is approximately 1/γ as illustrated in Fig. 3.1b.
The synchrotron source is not continuous, instead the electrons are bunched into packets atthe nodes of the accelerating radio-frequency field. For example, at the Advanced Light source
in Berkeley, the electron pack is about 35 ps and circulates at 55 MHz [37]. To achieve shorter
electron pulses, ultrafast optical lasers have been used to modulate the energy of a small slice of

11the electron packet [38]. The modulated electrons can then be spatially separated using bending
magnetics and apertures, resulting in pulse widths of 100’s of femtoseconds [39].

3.1.2

X-ray Free-Electron Lasers

In most laser gain media, the electrons are bound to atoms or molecules which limits typical gain media to the infrared, visible, and ultraviolet regions of the electromagnetic spectrum(Fig. 2.2). The Free-Electron Laser (FEL) is unlike typical gain media because the electrons areunbounded allowing great tunability from microwave to x-ray wavelengths. In a FEL, relativistic
electrons are passed through a series of magnetics, an undulator (see Fig. 3.2), which cause theelectrons to oscillate because of the Lorentz force. The oscillating relativistic electrons can emit
microwave to x-ray radiation. 1
The first theoretical consideration of radiation from relativistic electrons in a oscillating
magnetic field was done my H. Motz in 1951 [47]. Shortly after this theoretical prediction, in
1953, the first demonstration of radiation from an undulator was demonstrated [48]. However, thisdemonstration emitted incoherent light and thus could not be called a laser (it was also before theinvention of the laser so the term “laser” would not have been used anyway). The modern idea of a
FEL, as well as the term FEL, first appeared in a theoretical paper in 1971 by J.M.J. Madey [49].
J.M.J. Madey et al. realized the first observation of gain with an undulator structure in 1976 andthen the first FEL in 1977 [50, 51].
The key to producing short wavelengths is electrons traveling at nearly the speed of light.
When relativistic electrons pass through the undulator with a period of λu , the electrons “see a0Lorentz contracted undulator period λu = λu/γ , where γ is the relativistic factor given by
1γ=p

1 − v2/c2(3.3)

with v the velocity of the electrons in the lab frame and c the speed of light. The prime designatesa frame moving with the electrons. The Lorentz contraction is just one effect from the relativistic
1

For further Refs. see [40–46]

12speeds, another is the Doppler shift. In the lab frame, the light is blue shiftedω = γω 0 (1 + v/c)

(3.4)

where ω is the angular frequency in the lab frame. At this point a calculation can show, to firstorder, how short wavelengths of light can be generated from FELs. To begin, the undulator period
in the electrons frame is converted into angular frequency.
ω 0 = 2π

c
λ0u

(3.5)

From here the Lorentz contracted undulator period, λ0u , is transformed into the lab frame, λu .
ω 0 = 2π

cγ
λu

(3.6)

The angular frequency of radiation in the lab frame is given by,ω = 2πc γ2(1 + v/c).
λ0u

(3.7)

Changing the angular frequency to wavelength leads to,
λl =

λu
,
2
γ (1 + v/c)

(3.8)

where λl is the wavelength of emitted radiation as seen in the lab frame. Approximating v/c ≈ 1
because the electrons travel at nearly the speed of light results in
λl =

λu
.
2γ 2

(3.9)

a first order approximation of the wavelength emitted by an FEL. Plugging in modest parameters
for the LCLS facility in California, with as an undulator period of 3cm and a γ of 7800, the FEL
can produce 2.5 Å radiation [52].

3.2

Tabletop Sources
The large scale sources are impressive facilities but they are very expensive (100’s of millions

USD) and are limited to a few users at a time. Tabletop sources can complement large scale
facilitates because they are much smaller and cheaper (≈ 100-1000k USD) allowing table top sources
to be more available to university and industry laboratories.

13

Figure 3.2: Free-Electron Laser Relativistic electrons are passed through an area of alternating
magnetic fields. The magnetic fields cause the electrons to wiggle and as they wiggle they emit
radiation. The electrons are removed from the beam of radiation using a bending magnetic. Figure
adapted from Ref. [53].

14
3.2.1

EUV Lasers

The principle behind EUV lasers, just like optical lasers, is stimulated emission between
atomic levels. The first demonstration of EUV lasing, performed at the large-scale Novette laser
facility at Lawrence Livermore National Lab, used the transition between 2p5 3p and 2p5 3s in neonlike selenium [54]. Using a high-powered optical laser at 532 nm with 5 × 1013 W//cm2 , the target isionized by a line focus. Some of the emission from the excited selenium target travels along the longaxis of the plasma created by the line focus. The spontaneous emission simulates more emission as
is propagates along the plasma creating Amplified Stimulated Emission (ASE). In a typical opticallaser, the ASE will pass through the gain medium several times in a cavity configuration resulting
in large gains and high-coherence. However, due to the short lifetimes of the excited states requiredfor EUV lasing, multiple passes is not possible. Instead, EUV lasers use a single or double pass,thus resulting in lower coherence than cavity type lasers [55].
It was almost a decade until the first demonstration of tabletop EUV lasing because of theunfavorable pump density scaling. It takes a lot of pumping to create the exited states for EUV
lasing with the pump density, P , scaling as P ∝ λ15 . The first tabletop demonstration did not use
optical pumping, but instead an electrical discharge of 40kA in Argon gas [56]. Work has continued
to make the tabletop sources smaller and with faster repetition rates [57]. And today, even withthe unfavorable scaling, wavelengths as short as 8nm have been demonstrated using optical lasers
as the pump with picosecond pulse durations [58].

3.2.2

High-Harmonic Generation

The high-harmonic generation (HHG) process is a highly non-linear up-conversion of an
intense driving laser. The first HHG demonstration, in 1983, focused a 248.4 nm laser into heliumand observed the 7th harmonic at 35.5 nm [59]. The extension to ever higher harmonics, using
driving lasers with intensity’s of 1015 − 1016 W/cm2 , witnessed the 17th harmonic in Ne, again witha 248.4nm laser [60]. After the experimental demonstration, theory papers discussed the scaling of

15
HHG [61, 62], with the maximum energy from HHG given byhνcutof f = Ip + 3.17Up(3.10)

where h is Planks constant, ν is the frequency, Ip is the ionization potential of the atom, and U p is
ponderomotive energy [62,63]. The ponderomotive energy is the mean kinetic energy gained by thefree electron in the laser field and is proportional to Up ∝ IL λ2L where IL and λL are the intensity
and wavelength of the driving laser. As the harmonic cutoff suggests, higher energy photons are
generated with longer wavelength driving lasers because the longer the driving laser wavelength,
the longer the electron is accelerated in the laser field. The push toward bright keV photons is acurrent area of research [63, 64]. The work here used high-harmonics from an ultrafast Ti:Sapphirelaser. Further details on high-harmonic generation are discussed in Ch. 4.

Chapter 4

High-Harmonic Generation

Most of the work in this thesis was demonstrated with EUV light from a high-harmonicsource, with one exception of a benchtop HeNe laser prototype. High-harmonic generation (HHG)
is a highly-nonlinear process in which intense, ultrafast, laser pulses are up converted into the EUV
and the soft-x-ray spectral regions [63, 64].

4.1

Driving Laser
The driving laser for the HHG in this work uses a titanium doped sapphire crystal. In theearly 1990s, the broad bandwidth of Ti:Sapphire was harnessed in a mode-locked ultrafast laser [65].
The mode-locking in this laser uses the Kerr effect: a change in the refractive index due to intenseradiation. The laser cavity can be designed to use the Kerr effect, and when aligned properly, thecavity gain favors pulsed operation instead of a continuous wave. An example of the cavity of amode-locked laser, called an oscillator, is shown in Fig. 4.1.
The first demonstration had 60 fs pulses and subsequent work, reducing the cavity dispersion
with prisms, reduced the pulse length to 10 fs [67]. While the pulse length of the mode-locked
Ti:Sapphire is fast, the intensity of the pulse is not sufficient for high-harmonic generation. To
increase the intensity, the pulse must be amplified, but care must be taken because intense femtosecond pulses can burn optics or create non-linear effects in the cavity and thereby limiting thegain.
To amplify the short pulses by many orders of magnitude, chirped pulse amplification (CPA)17

Figure 4.1: Mode-locked laser cavity alignment This work used a mode-locked Ti:Sapphirelaser to seed an amplifier. The distances are as follows: a ∼ 62 cm, b ∼ 10.4 cm, θ ∼ 16◦ , c ∼22 cm, with the total prism separation (d+e) ∼ 62 cm, and f ∼ 5 cm. Figure adapted from Lytle
Ref. [66].

18

Figure 4.2: Chirped Pulsed Amplification Using chirped pulsed amplification, the seed pulse
from the oscillator, Fig. 4.1, is amplified to drive the high-harmonic generation process. Figure
adapted from Seaberg and Backus et al. Ref. [72, 74].

is used [68,69]. In CPA, the pulse is first stretched out in time using a grating system configured for
positive dispersion. Stretching the pulse to a 100 ps or more allows for relatively safe amplification,
as long as the optics are clean and have high-damage threshold coatings. In the laser system used inthis work, a KM Labs Dragon, the Ti:Sapphire crystal in the amplifier cavity is pumped with a 532
nm, frequency-doubled Nd:YAG, laser at 3-5kHz. The pumping laser (Lee Laser LDP-200MQGHP) can have an output as high as 100 W. This much power cannot normally be used to pumpbecause thermal lensing effects. However, this laser used cryogenic-cooling to reduce the thermal
lensing by two orders of magnitude [70]. After 12-13 passes through the amplifying crystal, thepulse is recompressed [71] to a 21-24 fs pulses [72, 73]. After the amplifier, the output at 3kHz has
about 3 mJ per pulse and is sufficient for high-harmonic generation. A schematic of the amplifier
is shown in Fig. 4.2.

4.2

HHG - The Microscopic Picture
In typical non-linear processes, like second harmonic generation, a driving laser field passes

through a material and the electrons are driven hard enough such that the harmonic-oscillator
potential is distorted and the material emits radiation at higher frequencies above the fundamental.

19
Taking this process to the extreme results in HHG [75].
For the HHG process to occur, the laser field needs to be intense, 1013 – 1016 W/cm2 such thatthe electron is ionized. While HHG has been demonstrated with solid [76] and plasma targets [77],we restrict our discussion here to HHG in a dilute gas [78].
In a semi-classical approximation (see Fig. 4.3), when the electron is tunnel ionized fromits parent atom, it is assumed to be in vacuum at zero velocity. However, the instant the electronis freed it is accelerated by the inhomogeneous electromagnetic field through the ponderomotive
force. When the oscillating laser field switches directions, and if the electron recombines with its
parent atom, the energy gained by the electron is released as a high energy photon. The maximum
energy that can be released is given by
Ecutof f = Ip + 3.2Up(4.1)

where Ip is the ionization potential of the atom and Up is the ponderomotive energy given byUp =e2 E 2
∝ Iλ2
4mω 2

(4.2)

where e and m are the electron’s charge and mass, E, ω, I, and λ are the laser fields amplitude,angular frequency, intensity and wavelength.
To extend the cutoff energy, Eq. 4.1, higher energy radiation can be produced from longer
wavelength driving lasers. The use of infrared driving lasers has generated photon energies in thewater window [79] and beyond, up to 1.4 keV energies corresponding to wavelengths shorter than
a nanometer [63]. Such high energies are the result of over 5000 infrared photons combining to
produce a single soft-x-ray photon.

4.3

HHG - The Macroscopic Picture
For a bright source of high-harmonic radiation, the high-energy photons emitted by individual

atoms need to constructively interfere. Constructive interference occurs when the phase velocityof the driving laser, νω , matches the phase velocity of the high-harmonic radiation, νqω , where q is

20

Figure 4.3: HHG - The Microscopic Picture An intense, ultrafast, laser is focused into a dilutegas. The laser field tunnel ionizes an electron and the freed electron is first accelerated away fromits parent atom before the oscillating laser field switches direction. Then the electron is driven
back to its parent atom where it recombines and releases its energy in a high energy photon. The
blue curves depict the wave packet evolution of the free electron along a classical trajectory. Figure
adapted from Ref. [75].

21
the harmonic order and ω is the fundamental angular frequency. For phase matching to occur, thedifference in wavenumbers, k = ω/νp , between fundamental driving laser, kω , and the high-harmonic,kqω , must be zero.
∆k = kqω − qkω = 0(4.3)

Coherent buildup of HHG in a dilute gas can be accomplished in a waveguide (see Fig.
4.4) [80–83]. In the waveguide, the dispersion can be described by three terms [84]: dispersion fromthe geometry, plasma, and free-electrons. The mismatch in dispersion is given byµ2 λL
2π∆k ≈ q 11 2 − qp(1 − η) (∆δ + n2 ) + qpηNa re λL
4πaλL| {z }|{z}| {z }
atoms
geometric
free-electrons(4.4)

where µ11 is the mode factor, a is the waveguide radius, η is the ionization level, re is the classicalelectron radius, Na is the number density of atoms/atm, ∆δ is the difference in the indices ofrefraction of the gas at the fundamental and x-ray wavelength, ω and λL are the fundamental laser
frequency and wavelength, n2 is the nonlinear index of refraction at λL for the given intensity(n2 = ñ2 IL ), IL , of the driving laser, and p is the pressure.
The sign of dispersion is positive for the geometrical and free-electrons, but negative forthe neutral atoms. Furthermore, the dispersion terms for the neutral atoms and free-electrons
are pressure dependent. By tuning the pressure in the waveguide, a balance of the dispersion
terms is possible resulting in a bright and coherent buildup of high-harmonic radiation. Typicalconversion efficiencies for HHG in a waveguide are on the order of 10−6 [66] and results in > 109
photons/sec/1% bandwidth [85].

4.4

Temporal Characteristics
As mentioned above, intense, ultrafast, laser fields are needed to generate high-harmonic

radiation. The ionization and recombination of the electrons occurs within the temporal envelopeof a single laser pulse, thus the high-harmonic radiation is also an ultrafast pulse. Typically, the√pulse width of the harmonic generation is given by τ/ 2, where τ is the driving laser pulse width22

Figure 4.4: HHG - The Macroscopic Picture An intense, ultrafast, laser is focused into
waveguide. The gas pressure in the waveguide is tuned achieve phase matching. This results in a coherent addition of the high-harmonic radiation. Figure courtesy of KM group(https://jila.colorado.edu/kmgroup/research/articles/attosecond-nonlinear-optics).

23
and q is the harmonic order [86].
There are a couple of methods to generate high-harmonics such that the bust of radiation
occurs on attosecond (as) time scales.1

One method uses polarization gating, such that thedriving laser has a phase locked polarization modulation which only permits the generation ofhigh-harmonics within a single-cycle resulting in 130 as pulses [87]. In an alternative method, theintensity of the laser can be tuned, such that the generation of high-harmonics is achieved only
during the most intense single-cycle of the driving laser [88]. Using mid-IR driving lasers, soft-xray bursts of high-harmonics have been demonstrated [89]. The combination of short wavelength
radiation, ultrafast bursts, an inherently synchronized pulses with the driving laser, makes HHG
the ideal source for imaging at the spatiotemporal limit using pump-probe methodologies. Next,
imaging forming methods with EUV and x-rays are discussed.

1

A review on attosecond pulse generation [30].

Chapter 5

Imaging Forming Methods with EUV and X-rays

Probably the simplest method to form an image with EUV and x-rays is to record the shadowof the object, as done in medical x-ray imaging (radiography). Radiography provides information
about the distribution of absorbing materials with resolution on the order of millimeters. The
sensitivity of radiography can be improved with phase enhancement approaches [90], but the resolution is not improved because no images are formed. The ability to from images in the EUV/x-ray
region is not as straightforward as imaging with optical wavelength because of the lack of suitablerefractive lens elements, with one exception: the compound refractive lens [91–93].
Recently, compound refractive lens elements have been developed to focus x-ray radiation toabout 100 nm spot sizes [94]. A series of cylindrical or parabolic holes in low-z materials such as
beryllium, act as lenses in the hard x-ray regime (see Fig. 5.1). The focal length, F , of these lenses
is given by
F =

R
2N δ

(5.1)

where R is the radius of the hole in the material, N is the number of holes, and δ is the decrementof the refractive index n (n = 1 − δ). For now, compound lenses are suitable for hard-rays, because
as of yet, no suitable material has been found to work in the EUV spectral region.
A couple of methods to improve the resolution of x-ray imaging, without lenses (compoundor otherwise), use small apertures. In the first method, the aperture is placed directly in frontof the sample and is then raster scanned. The transmitted light at each position is summed ona detector, thus forming an image of the sample with the resolution dependent on the size of the25

Figure 5.1: Compound Refractive Lens The compound lens consists of holes fabricated into a
low-z material. Depicted here is the focal length of the compound refractive lens given in Eq. 5.1.
The focal length is dependent the radius of the hole, R, the decrement of the refractive index, δ,and the number, N , of holes. The spacing, d, between the holes in not critical to the design. This
figure is adapted from Ref. [95].

26
aperture [96]. The second method, requires a coherent beam. An aperture next to the sample
can be used a reference beam for Fourier transform holography [97] as depicted in Fig. 5.2. In
Fourier transform holography, the scattered light from the reference pinhole interferes with thescattered light from the sample. The interference is encoded at the detector plane by intensity
modulations and by taking the Fourier transform of the recorded diffraction pattern, an image ofthe sample is retrieved. Fourier transform holography has been used to image magnetic structuresusing circularly-polarized light from synchrotrons with 50 nm resolution [98]. The resolution of
Fourier transform holography is dependent of the size of the aperture. Increasing the resolution
is challenging because as the aperture is decreased, more and more photons are blocked, thus
becoming increasingly more photon inefficient.
The application of mirrors to x-rays was pioneered at Stanford by Kirkpatrick and Baez [99].
They used super polished substrates placed at 90 degrees with respect to each other, each witheither a parabolic or elliptical curvature (see Fig. 5.3a). The curved substrates are able to focus aglancing incident x-ray beam and are known as K-B mirrors. The glancing incident angle is needed
for high reflectivity. Another mirror geometry, the Schwarzschild configuration, uses sphericalmirrors to focus the beam (see Fig. 5.3b) [100, 101]. The use of two mirrors in a proper design,
can reduce the astigmatism from spherical surfaces [102, 103]. Due to the near normal angle ofincidence in the Schwarzschild configuration, they are typically used in EUV applications withmultilayer mirrors. Multilayer mirrors are layered structures designed such that a select bandwidthof radiation is reflected. The surface quality of the mirrors tend to limit resolution to about
100nm [104]. However, recent work using deformable mirrors, has improved the focal spot toaround 10nm [105].
Mirrors do not require coherence, but the follow optics due require a coherent beam: theFresnel zone plate and Laue lens. The Fresnel zone plate is a series of rings, designed such thatsome of the diffraction is focused to a spot (see Fig. 5.3c). The resolution from a zone plate isdependent on its fabrication quality, especially the width of the outer most ring. Similar to the zone
plate, is the Laue lens (see Fig. 5.3d) [106]. The Laue lens can be thought of a one dimensional zone

27

Figure 5.2: Fourier Transform Holography In Fourier transform holography, a small aperture is fabricated near the sample. The aperture creates a reference beam that interferes withthe diffraction from the adjacent sample. The interference is recorded on a detector as intensity
modulations. A Fourier Transform of the intensity results in an image of the sample. In the work
depicted here, the sample consists of magnetic domains. Figure adapted from Ref. [98].

28
plate, creating a tight focus in one-dimension, as tight as 8nm [107]. The Laue lens is created with
sputtering methods, as opposed to e-beam lithography techniques used in zone plate fabrication,
allowing for 1 nm layers [108]. The ability to make thinner layer promises to further improve thespot size of the Laue lens because, like the zone plate, the resolution is dependent on the layer
thickness.
The ability to focus x-rays leads to point scanning imaging forming methods. Point scanning microscopy techniques with zone plates have achieved 30nm resolution [109, 110], while direct
imaging with zone plates have achieved 15, 12, and 10 nm resolution [111–113]. A combination ofK-B mirrors and zone plates has recently demonstrated 5nm spot sizes [114], which is promising for
future high-resolution imaging. Furthermore, by analyzing the intensity changes between adjacentpoints, quantitative phase information is possible [115].1
The imaging forming techniques used in this work do not require any image forming optics,
thus the resolution is not dependent on fabrication quality. Furthermore, because no optics areneeded between the sample and the detector, this technique is the most photon efficient form ofimaging [117]. The resolution in this technique is not dependent on any apertures or pinholes,
thus resolution is only limited by Abbe’s diffraction limit (Eq. 2.2). This technique is not a point
scanning technique, therefore large areas can be imaged in a single exposure. And finally, thistechnique is a full characterization of how light interacts with the sample yielding both amplitude
and phase information. The technique used in this work is coherent diffractive imaging.
Coherent diffractive imaging (CDI), was adapted to optical problems from the GerchbergSaxton algorithm [118] used in electron microscopy, in 1978 by Fienup [119,120]. 2 At first this newimaging technique was limited to computer simulation, until the first demonstration with opticalbeams in 1988 and 1990 [122, 123]. It was a decade later, in 1999, that the first demonstrations of
CDI were demonstrated using x-rays in 1D by Robinson et al. [124] and 2D by Miao et al. [125].
With all the advantages of CDI, there also comes some challenges. The experimental con1
2

A nice review on non-CDI imaging [116].
A history of CDI is found in [121].

29
straints and requirements for CDI are discussed in Ch. 6. Overcoming some of those challenges is
one aspect of these thesis work and is discussed in Chs. 7 and 8. And finally, extending CDI for
stroboscopic dynamic studies is discussed in Ch. 9.

Figure 5.3: Various EUV and X-ray Optical Elements (a) The Kirkpatrick-Baez mirror
which consists of two super polished substrates with parabolic or elliptical curvature for hard x-ray
focusing. Panel adapted from Ref. [126]. (b) The Schwarzschild objective consists of two sphericalmirrors, typically multilayer mirrors, and used in the EUV. Panel adapted from Ref. [101]. (c)The Fresnel zone plate is a diffractive element consisting of concentric rings. Panel adapted from
Ref. [127]. (d) The Laue Lens is a diffractive element which can form a line focus from sputteredlayers of materials. Panel adapted from Ref. [106].

Chapter 6

Coherent Diffractive Imaging

The objective of CDI can be stated as follows: given a diffraction pattern from an unknown
object, reconstruct the object. If the phase could be measured on a detector, the recovery of theobject would be a simple inverse Fourier transform (see appendix A for a discussion the applicabilityof the Fourier transform). Unfortunately, the phase is lost by the detector and various methods ofphase retrieval must be employed.1

6.1

History of Phase Retrieval
In 1952, Sayre [130] noted Shannons sampling theory [131] may lead to a solution to thephase retrieval problem if the diffraction pattern could be sufficiently sampled. Twenty years
later, Gerchberg and Saxton developed the first widely used algorithm for phase retrieval [118].
This algorithm used the diffracted amplitude and an image of the object to solve for the phase.
Because an image of the object is required, this algorithm in not suitable for a CDI microscope
when the sample is unknown. In 1978, Fienup built upon the Gerchberg-Saxton algorithm witha modification of the image constraint [119]. Instead of an image of the object, the object mustbe isolated and this algorithm was termed Error Reduction (see Fig. 6.1). The isolated object, or
support constraint, is motivated and discussed in more detail in Sec. 6.2. Since Fienup’s initial
CDI algorithm, the CDI community has worked to improve phase retrieval algorithms with respect
to convergence speed and robustness to noise. [120, 132–136].
1

For review articles see Refs. [128, 129]

31
A notable example is the shrink-wrap algorithm put forward by Marchesini et al. in 2003 [133].
Before the shrink-wrap algorithm, the support constraint was applied like it is depicted in Fig. 6.1c:the same shape at each iteration even if the object is converging to a smaller sub-region. The shrinkwrap algorithm uses a blurred and thresholded version of the object, before the support constraint(Fig. 6.1b), as the isolation constraint. The shrinking support constraint leads to faster convergenceand reduces stagnation problems of phase retrieval algorithms.

6.2

Oversampling and the Isolation Constraint
From Shannon’s seminal paper on sampling theory [131], bandlimited, or isolated samples,

if sampled at the Nyquist frequency, can be recovered exactly from their Fourier transform [138].
This is only true if the phase is known. Without the phase the diffraction amplitude must be
sampled at greater than the Nyquist frequency.
Consider the phase retrieval problem as a set of linear of equations with known and unknown
pixel values. The amplitude of the Fourier transform of the object is measured on a N × N pixel
detector in frequency space (see Fig. 6.2). From the measurement of the Fourier transform, we
have N 2 known data points. In object space, without the isolation constraint, we have N 2 unknown
amplitude and N 2 phase points for a total of 2N 2 unknowns. This does not have a unique solution.
To solve the problem, there must be a constraint to limit the number of unknowns. If we√√

restrict the object to a square region of N/ 2 × N/ 2 then the number of unknowns becomes N 2/2
amplitude and N 2/2 phase points for a total of N 2 unknowns. Now the number of know and unknown
pixels are the same allowing a unique solution. The isolation constraint in object space corresponds
to a diffraction amplitude pattern that is sampled at greater than the Nyquist frequency leading
to the so-called oversampling ratio [139–142], σ, which can be written asσ=total pixel number.
unknown-valued pixel number(6.1)

A theoretical oversampling ratio of 2 is required and this requirement corresponds to oversampling√by > 2 in each dimension for a 2D object [140]. In practice, it is best to have a ratio of 4 or an

32

Figure 6.1: CDI with Error-Reduction (a) A measured diffraction pattern is fed into the algorithm and random phase guess is applied. (b) The diffraction in (a) is inverse Fourier transformed
into object space. (c) The isolation constraint or support is applied. (d) Application of the support
constraint yields a better guess of the object. (e) The better object guess in (d) is Fourier transformed back to frequency space. Here the phase is kept, but the amplitude is replaced with themeasured amplitude. Convergence of the algorithm can be monitored by calculating the difference
between (e) and (a). The algorithm continues to loop until some termination condition is met suchas an error below a predefined threshold. Figure panels contain data from Ref. [137].

33

Figure 6.2: Oversampling and a Isolated Object (Top) A Nyquist sampled diffraction pattern, when inversed transformed, results in a object that fills the gird. (Bottom) An oversampled
diffraction pattern, when inversed transformed, results in an isolated object. Figure adapted from
Ref. [139].

34
oversampling of 2 in each dimension to overcome noise in the measurements.
For convenience, the oversampling ratio can be re-written using tunable experimental parameters
σ≥2=

N
N/2

=

N dx
D

(6.2)

where dx is the object pixel size and D is the largest extent of the sample. The object pixel size isrelated to the detecotor pixel size by Fourier relationships [138]
dx =

λz
N px

(6.3)

where λ is the wavelength of illumination, z is the distance from the sample to the detector, andpx is the pixel size of the detector. Plugging Eq. 6.3 into Eq. 6.2 yields
σ=

λz
≥2
D px

(6.4)

a very useful expression when designing a CDI microscope.

6.3

Ptychography
Ptychography is a powerful CDI technique based on many diffraction measurements fromthe sample. The sample is illuminated and is scanned, area-by-area, with about 60%-70% overlap
between adjacent scan positions. From the set of diffraction patterns, and the known shifts between
scan positions, it is possible to reconstruct both the amplitude and phase of the sample.

6.3.1

History

Ptychography started with theoretical investigations of phase retrieval for crystalline samples[143] using the convolution theorem of Fourier optics [138].2

The early work was published inGerman, in which the German word for convolution is word for folding [145]. Following scientificnaming conventions, the Greek work of fold is ptycho, hence the name ptychography.
The early description of ptychography considered a crystalline sample illuminated with afocused beam from a lens with a hard aperture. The diffraction pattern, using the convolution
2

The discussion here is presented in greater detail in Refs. [144, 145]

35
theorem, is the Bragg peaks of the crystal diffraction convolved with the Fourier transform of the
focused beam. Hoppe realized the phase could be retrieved by measuring the intensities of two
adjacent diffraction orders and their interference fringes. At the time of the early ptychography
work, coherent sources in the EUV and x-ray spectral regions were not fully developed and thus it
was some time before ptychography became widely used.
Ptychography was developed for non-periodic objects in the 1990s [146]. It was realized thatthe resolution in a scanning microscope is not necessarily dependent on the focus spot size. Instead,collecting the diffraction patterns and using a Wigner deconvolution, the resolution is proportional
to the scan step size as opposed to the spot size [145]. This early experimental work was able todecouple effects from the illuminating and improved the resolution of scanning microscopy, but theentire dataset needed to be deconvolved at once. This was not easily done at the time given thelack of computer resources to handle such large datasets.
A beakthrough in ptychography occurred in the early 2000s [147, 148]. Instead of using theentire dataset at once, as in the Wigner deconvolution method, one diffraction pattern can beconsidered at a time. In combination with phase retrieval methods pioneered earlier by Fienup[119, 120], each diffraction could be considered serially with the object updated piecemeal. With
overlap from adjacent scan positions, ptychography has more constraints than traditional CDI. The
first methods of serial ptychography required accurate knowledge of the illumination, but works in2008 and 2009 further improved the ptychography algorithm to solve for both the object and theillumination [149, 150].

6.3.2

Ptychographic Data Collection

Here we address ptychography using EUV and x-ray sources, although the same considerations apply to other coherent sources (such as some forms of electron microscopy [151, 152]). We
assume that the illumination is sufficiently coherent and monochromatic [153]. We also consider
the thin sample approximation [149] applies to our case of study, such that the interaction of probe36
and the sample can be described by:ψ(~r) = O(~r)P (~r)(6.5)

where ψ is the exit-surface wave (ESW), O is the complex-valued object, P is the complex-valued
probe, and ~r is the real space coordinate vector. We further assume that propagation from the
ESW to the detector plane can be described with a propagator, F, and an inverse propagator, F−1 ,such that (see appendix A for a discussion):ψ(~r) = F−1 [Ψ(~u)] = F−1 [F[ψ(~r)]](6.6)

where Ψ is the ESW at detector and ~u is the spatial frequency coordinate vector. In many instances,the propagator is the Fourier transform because the detector is placed sufficiently far from thesample such that the far field approximation is satisfied:
W2
<< 1
zλ

(6.7)

where W is the diameter of the area illuminated on the sample, z is the distance from the sample
to detector plane, and λ is the wavelength of illumination. The detector records the intensity, I, ofthe diffracted light given by I(~u) = |Ψ(~u)|2 . As discussed in 6.2, the geometry of the data collectionneeds to ensure oversampling of the diffraction [140].
A ptychographic dataset consists of scanning the probe over the object at j known positions,r1 , r2 , r3 ,...,rj , yielding a set of intensity measurements:
Ij (~u) = |F[O(~r)P (~r − rj )]|2

(6.8)

where rj is a shift transverse to the beam direction and the | | indicate the absolute value. At
each scan position, the illuminated portion of the sample overlaps with adjacent scan positions.
For a robust reconstruction, 60% − 70% overlap is typical between adjacent scan positions [150].
A useful chart for ptychographic data collection is shown in Fig. 6.3. Assuming the illumination
is a uniform circle, Fig. 6.3 shows the overlap of adjacent position as a function of radius, R. For
an overlap of about 70%, the illumination needs to be shifted by R/2. For the work in this thesis,

37
shifts of R/2 are considered a minimum threshold of overlap. Most ptychographic datasets had
R/3 or R/4 overlap because the redundant information allows the algorithm to be more robust in
the presence of noise. However, too much overlap can be a problem, because the diversity in thediffraction patterns decreases resulting in a stagnation of convergence. To overcome the lack ofdiversity in the diffraction patterns, a large scan is needed.
When scanning the sample in a rectilinear grid, artifacts from the periodic scan grid may beintroduced into the reconstruction [154]. To avoid this, each scan step is randomly offset by up to
20% of its step size. This is the so-called noisy grid scan pattern. Its been shown the best scanpattern is a Fermat spiral because there is uniform illumination without periodicity [155].

6.3.3

The Ptychography Algorithm

The ptychography algorithm starts with the ESW from an object and probe guess such that
ψGj (~r) = OG (~r)PG (~r − rj )(6.9)

where the subscript G designates a guess. Typically the initial guess of the object is unity; the probe
is an estimate of the illumination based on a size or better yet, a calculation of the illumination
at the sample through all the optical components upstream. The ESW guess is propagated to thedetector, forming a guess of the diffractionΨGj (~u) = F[ψGj (~r](6.10)The recorded diffraction pattern, I(~u), at the position rj , is used to constrain the algorithm withthe modulus constraint, M , expressed as
ΨM j (~u) =

p

I(~u)

ΨGj (~u)|ΨGj (~u)|(6.11)

where ΨM j (~u) is the diffraction at the detector plane, consistent with the measured diffraction,
which also contains a guess of the phase. The diffraction, ΨM j (~u), is propagated back to the
0 (~sample plane forming a better guess, ψGjr) = F−1 [ΨM j (~u)], of the ESW because the ESW is now

consistent with the measured diffraction.

38

Figure 6.3: Overlap and Probe Shifts Assuming the illumination (probe) is a uniform circle,
this graph shows the overlap of adjacent scan positions as a function of shift. The vertical axis
is the amount of overlap in percentage and the horizontal axis is the probe shift in units of circle
radius R.

39
At this point, the object and probe guesses are updated employing the known overlap between
adjacent positions. The particular form of the update varies between algorithms, see for example
Refs. [149, 150, 154, 156–158]. The ptychography reconstructions in this work are based on theextended ptychographical iterative engine (ePIE) algorithm [150]. In this algorithm the object
guess, OGj (~r), and the probe guess, PGj (~r − rj ) , are updated by the following equations:
OGj+1 (~r) = OGj (~r) + α

PGj+1 (~r) = PGj (~r) + β

∗ (~
PGj
r − rj )|PGj (~r − rj )|2max

∗ (~
OGj
r + rj )|OGj (~r + rj )|2max0(ψGj(~r) − ψGj (~r))(6.12)0(ψGj(~r) − ψGj (~r))(6.13)

where α and β are feedback parameters and ∗ denotes the complex conjugate. The feedback
parameters in this work are unity. These better guesses, OGj+1 (~r) and PGj+1 (~r), are be fed backinto the algorithm until all j positions have been updated. At this point, one full iteration of
ptychography is complete. Further iterations of ptychography will continue following the described
iterative procedure, until a convergence condition is met, which usually consists of a minimizationof an error metric [159]. A flow chart of ptychography is shown in Fig. 6.4. Having described CDI,
its application to EUV and and specially in a reflection geometry is discussed next.
-

40

Figure 6.4: Ptychography data collection and flowchart The ptychographic dataset consistsof a set of diffraction patterns collected at known object shift positions. The dataset is fed into theptychography algorithm and which solves for both the object and the probe.

Chapter 7

Coherent Diffractive Imaging in a Reflection Geometry

As discussed previously, coherent diffractive imaging (CDI) is a promising solution for EUV
and x-rays imaging because the resolution scales with the wavelength. Nearly all of the EUV
and x-ray CDI demonstrations to date have been in a transmission geometry, with only a few
exceptions [160–164]. None of the previous works have been able to obtain near wavelength limited
resolutions which is needed to image nanostructures patterned on substrates, substrates that are
too thick for transmission imaging.
This chapter is divided into two sections. In the first section, a benchtop optical CDI microscope is developed, using a 632 nm Helium Neon laser, to rapidly iterate solutions for reflection mode
imaging. An algorithm was developed, named tilted plane correction, which enabled high-fidelity
reconstructions. The application of tilted plane correction using 30 nm high-harmonic radiation,is the topic of the second half of this chapter. The highest resolution-to-wavelength images wereobtained in the EUV and x-ray spectral regions using CDI in this work.

7.1

Aperture-Illumination Coherent Diffractive Imaging
Interestingly, the application of CDI, using light sources in any region of the electromagnetic

spectrum, has been limited almost exclusively to transmission mode imaging (at the time of thiswork in 2012), with the exception of two recent experiments [160, 161]. This is due to the factthat reflection mode geometries are intrinsically more demanding than transmission mode samples
since it is far more difficult to isolate the sample. Marathe et al., Ref. [160], isolated the object by42
placing a pinhole directly onto the sample. While this simplistic approach works for their micronscale samples, it will not work with sensitive nanoscale structures because the attachment of thepinhole will either damage or alter sensitive samples. Furthermore, their technique does not easily
allow imaging of different parts of the sample since the pinhole is attached directly to the sample.
In the work by Roy et al. [161], the pinhole was not placed on the sample, but instead placed
between the sample and detector. Unlike Ref. [160], the sample is unaltered and different areas canbe imaged, but the numerical aperture (NA) is severely limited. The reduction in NA limits theattainable resolution and therefore their resolution of 60nm is far from their wavelength of 2.5nm.
We demonstrate the most straightforward strategy for reflection mode CDI by simply illuminating the object with the image of a pinhole, an approach termed aperture-illumination CDI(AICDI). For the first time CDI can image and scan over large samples with high NA, in an off-axis
reflection geometry, demonstrating a versatile reflection mode microscope.1

7.1.1

Transmission mode AICDIIn order to implement and test the AICDI technique, and associated data processing algorithms, a proof-of-concept system is developed using a polarized 632.8 nm HeNe laser in a transmission geometry. A schematic diagram of the setup is shown in Fig. 7.1. The illuminated beam
overfills a 300 µm diameter circular aperture. The aperture is imaged to the sample plane using a
one-to-one 4f imaging system. A bundle of suspended 26 µm diameter copper wires in a crisscrosspattern across a half-inch diameter ring is used as the sample. The inset in Fig. 7.1 shows an
optical microscope image of the sample. A positive lens placed directly after the sample sends thescattered light into the Fourier plane at the CMOS detector (Mightex Systems MCE-B013, 5.2µm pixel size). In general, the positive lens after the sample is unnecessary, however the detector
used in this experiment has a small collection area, such that a demagnification of the far field was
required in order to use a wavelength as large as 633 nm. The aperture size is selected to satisfy
the oversampling criterion [139–142] ( see Sec. 6.2), where the distance between the lens and the1This section is adapted from Gardner et al. [165]43detector is 11.6 mm, corresponding to an NA 0f 0.22 for our 5.3 mm detector.
A bundle of suspended copper wires, 26µm diameter, were illuminated with an image ofthe aperture to demonstrate the effectiveness of this technique for imaging extended samples. An
optical microscope of the suspended wires is shown in Fig. 7.1. An example of a recorded diffraction
pattern is shown in Fig. 7.2a. We use the RAAR algorithm as outlined in Ref. [134] with shrinkwarp [133] to recover the phase. (An explanation of the shrink-wrap algorithm is given in 6.1).
With the recovered phase, we are able to reconstruct the exit surface wave as shown in Fig. 7.2b.
This technique constitutes a bright-field imaging microscope.
A dark-field image can be obtained, if instead the scattered light, with the sample removed(leaving the rest of the system unchanged), is measured. This measurement of the un-diffracted
illumination is used to reconstruct the electric field at the sample plane. During the reconstruction
process, the complex amplitude of the illumination at the detector plane is subtracted at each
iteration. Subtracting out the illumination results in the wires appearing bright instead of dark as
in Fig. 7.2c, and constitutes a dark-field microscope.
By scanning the sample in a plane perpendicular to the optical axis, we are able to reconstructdifferent areas of the extended sample independently. With overlap between the scan positions, we
can register adjacent reconstructions to build up a large-area, high resolution image. Figure 7.2dshows a number of reconstructions of this sample, which were overlaid in post-processing. Colored
circles indicate the area that was illuminated by the aperture for each individual reconstruction.

7.1.2

Reflection mode AICDIHaving shown the ability to isolate and image part of an extended sample in transmission,
AICDI is now applied to samples in a reflection geometry. Unless the detector has a hole foran illumination beam, the sample must be at some non-zero angle of incidence with respect tothe beam. At non-zero incidence angles, and at high NA, the far field diffraction pattern is nolonger proportional to a uniformly spaced Fourier transform of the specimen, as evidence by thecurvature of the diffraction pattern in Fig. 7.3a. A correction is needed to remap the diffraction

44

Figure 7.1: Aperture-Illumination Setup The illumination is passed through a pinhole apertureand then is imaged onto the sample plane. The inset shows an optical microscope image of thesample which consists of a crisscross pattern of 26 µm diameter wires. After the sample, a positive
lens is placed transforming the scattered light into the Fourier plane at the detector where thediffraction pattern is recorded. Figure adapted from Gardner et al. [165].

45

Figure 7.2: Aperture-Illumination Transmission Imaging (a) An example of the collecteddiffraction from the wire sample scaled by the 4th root. (b) The exit surface wave reconstructedfrom the diffraction pattern. The circle outlines the area illuminated by the aperture. (c) Areconstruction when the illumination is subtracted out. (d) Overlay of the images from many scan
positions. The circles represent the outline of the aperture illumination at different scan positions.
Figure adapted from Gardner et al. [165].

46

Figure 7.3: Tilted Plane Correction (a)The raw diffraction from light scatted by the sample
at an angle of 30 degrees (b) The data mapped onto a linear grid in frequency space. The dottedblack lines are added to highlight the curvature seen in the tilted sample diffraction shown in (a).
Both images have been scaled by the fourth root. Figure adapted from Gardner et al. [165].

onto a linearly spaced grid. This remapping, termed tilted-plane correction, is described in detailin appendix B and Ref. [165]. The application of titled-plane correction allows the use of theFast-Fourier transform (FFT) algorithm [166, 167]. The use of the FFT improves the speed of thealgorithms and allows the use of any of the existing phase retrieval algorithms.
To demonstrate the tilted-plane correction and reflection mode imaging, the transmission
system was modified so the sample was at an angle of θ = 30 degrees (Fig. 7.4a). The samedetector and Fourier transform lens were used as in the transmission setup, but were re-positioned
such that they were aligned along the specular reflection from the sample. The NA was kept at 0.22
and the resolution at 1.4µm. A positive 1951 Untied States Air Force (USAF) resolution target
was used as the sample. Figure 7.3a shows the diffraction pattern from the vertical bars of group 5(element 1) of the resolution target. The black dashed lines are overlaid to illustrate the curvaturein the diffraction resulting from the non-zero angle of incidence. In Fig. 7.3b, the re-mapped
diffraction onto a linear grid in spatial frequency is shown. After the interpolation of tilted-plane
correction, the diffraction pattern is proportional to the modulus of the Fourier transform of thesample. Using the same iterative phase retrieval algorithm as mention in section 7.1.1, the AICDI
technique is capable of reconstructing an arbitrary position of the target. Reconstructions are47
overlaid and shown in Fig. 7.4b. An objective based bright field microscopy image is shown in Fig.
7.4c for comparison.

7.2

Near-Wavelength Resolution CDI in Reflection with EUV
The above benchtop proof-of-principle demonstration of high-NA reflection CDI is now adaptedand applied to EUV radiation. A 30 nm high-harmonic beam is used to illuminate a titaniumpatterned silicon wafer in a reflection geometry. High quality, high contrast, full filed images are
retrieved using tilted plane correction and ptychography. Images with 80 nm by 40 nm lateral(1.3λ) resolution are obtained with quantitative phase information enabling profilometry with 6
angstrom (Å) resolution.2

7.2.1

High numerical aperture data collection of scattered EUV

Intense ultrashort pulses from a Ti:Sapphire laser amplifier system are used to generate thehigh-harmonic beams (see Ch. 4 for a discussion on high-harmonic generation). In this experiment,
the driving laser had a central wavelength of 780 nm, pulse energy of 1.4 mJ, and operated at a 5
kHz repetition rate with 22 fs pulses. The waveguide used to generate the harmonics was 200 µm
in diameter, 5 cm long, and filled with argon at 36 Torr backing pressure. After the waveguide,a differential pumping scheme is used to limit absorption of the EUV light and maintain highvacuum (10−6 Torr) is the experimental chamber. To remove the co-propagating driving laser fromthe harmonic radiation, a pair of silicon rejecter mirrors, set near Brewsters angle for 780 nm, isused with two 200 nm-thick aluminum filters.
Figure 7.5a depicts the inside of the experimental chamber where two 45◦ angle-of-incidence
multilayer mirrors select the 27th harmonic (28.8 nm). The harmonic beam is focused onto thesample using a nickel-coated ellipsoidal mirror with a 5◦ grazing incidence angle. The sample isplaced just after the focus of the ellipse, at an angle of 50.5◦ and the scattered light is recordedon an EUV-sensitive CCD with a square array of 2048 × 2048 pixels, each with a side-length of2This section adapted from Zhang and Gardner et al. [168].

48

Figure 7.4: Aperture-Illumination Reflection Imaging (a) A schematic of the setup. Notethat a negative USAF pattern is shown, but a positive USAF was used in the experiment. (b)Several images with different scan positions are overlaid to show the AICDI reconstructions. (c)A traditional bright-field microscopy image of the sample. The scale bar in (c) is shared with (b).
Figure adapted from Gardner et al. [165].

49
13.5 µm (Andor iKon-L). The CCD plane of the camera is placed 3.17 cm from the sample andperpendicular the specular reflection, resulting in a numerical aperture of 0.4. Figure 7.5b shows
an SEM image of the sample, consisting of titanium shapes patterned onto a silicon substrate using
e-beam lithography. This same sample was used in a previous experiment and details about the
fabrication can be found in the supplemental section of Ref. [169]. Due to the sample’s age and its
storage in a laboratory environment the surface of the sample was contaminated, which resulted
in very fine height variations across the sample. The fine variations on the sample are used, as
discussed below, to compare our CDI methods with SEM and AFM.
Before collecting the ptychographic dataset (see Sec. 6.3.3), the beam size at the sample
plane is measured using a knife-edge scan. The beam size diameter was measured to be 12 µm
in both the horizontal and vertical directions. With a step size of ≈ 3 µm, we ensure about
70% oversample between adjacent scan positions (see Fig. 6.3). The camera recorded diffraction
patterns from a total of 198 positions in a nearly rectangular scan grid of 18 × 11 points. To prevent
periodic artifacts from being introduced by the scan grid, random offsets up to 20% of the step
size are added before each step. Each collected diffraction pattern had an exposure of 0.1 s with 3
accumulations for a total exposure time of 59.4 seconds.

7.2.2

Reconstructing high-NA reflection geometry data using CDI

An example of a raw diffraction pattern from the sample is shown in Fig. 7.6a. The frequencies associated with the raw diffraction are mapped non-linearly onto the detector due to a
combination of the non-zero angle-of-incidence and the high NA data collection. In order to use
the fast Fourier transforms [166, 167] in our data analysis, the raw diffraction is re-mapped intolinear frequency using tilted plane correction [165,168,169]. The remapped, or corrected, diffraction
pattern is shown in Fig. 7.6b. As a result of the remapping, the NA in the x-direction (horizontal) is reduced compared with the y-direction (vertical). The diffraction patterns were cropped to
512 × 1024 pixels corresponding to a reconstruction pixel size of 76 nm in the x-direction and 38
nm in the y-direction.

50

Figure 7.5: High-NA reflection geometry and sample a) A depiction of the experimental
chamber showing high numerical aperture data collection of diffracted EUV light from the sample.
The multilayer mirrors select a single harmonic and the ellipsoidal mirror focus the EUV onto
the sample. b) A scanning electron microscope image of the sample, which consists of patternedtitanium shapes on a silicon wafer. Panel (a) is adapted from Zhang, Gardner et al. [168].

51

Figure 7.6: Tilted Plane Correction in the EUV a) Diffraction collected from the sample ina high-NA reflection geometry. The frequencies associated with the diffraction are mapped nonlinearly onto the detector. b) The remapped, or corrected, diffraction pattern. In the correcteddiffraction, the frequencies are linearly spaced. Figure adapted from Zhang, Gardner et al. [168].

52
A complex-valued image of the sample was reconstructed using the extended ptychographicaliterative engine (ePIE) algorithm [150] with position refinement [170]. The retrieved amplitude
and phase are shown in Fig. 7.7b,c with a SEM image for comparison in panel (a). The phase
information, Fig. 7.7c, is used to create the 3D rendering of the sample shown in Fig. 7.8.

7.2.3

Resolution Characterization

Three methods were used to characterize the lateral resolution: the phase retrieval transfer function [171, 172], the modulation transfer function (MTF), and a knife-edge test (10%-90%
width). All approaches to characterize the resolution, shown in appendix C, support a lateral
spatial resolution of 76 nm in the horizontal direction and 38 nm in the vertical direction.
The phase of the ptychographic reconstruction was converted to height using
φ=2π(2h cos θ)
λ

(7.1)

where φ is the reconstruction phase, λ is the wavelength of illumination, h is the sample height,and θ is the angle of incidence on the sample. To avoid 2π ambiguities or complex reflection
coefficients, only the heights of the substrate are compared with the AFM. The AFM image hada higher resolution than our ptychographic reconstruction, so a Gaussian blur was applied, suchthat the resolution is equivalent. After smoothing, the 2-σ (95% confidence interval) of a histogram
difference of the CDI calculated height and AFM profile is ≈ 6 Å.

53

Figure 7.7: High-Resolution EUV imaging in a reflection geometry a) Scanning electron
microscopy (SEM) image of the sample for comparison with ptychographic coherent diffractive
imaging (CDI) b) Amplitude and c) phase reconstruction. Figure adapted from Zhang, Gardner et
al. [168].

Figure 7.8: Three-Dimensional Rendering from the Phase Information Using the phase
information from the ptychographic reconstruction, a 3D rendering is generated. Figure courtesyof Dan Adams.

Chapter 8

Sub-wavelength coherent imaging of a periodic sample

Progress in algorithm development and computing, coupled with improvements in coherent
short wavelength light sources, are leading to revolutionary advances in coherent diffractive imaging(CDI) at extreme ultraviolet (EUV) and X-ray wavelengths. However, to date it has been challenging to obtain high-fidelity images of periodic objects using CDI because most of the diffraction
pattern is dominated by intense peaks from the underlying periodicity. In this chapter, a tabletop
13.5 nm high harmonic beam is used to make two significant advances: first, a demonstration ofhigh-quality imaging of an extended nearly-periodic sample for the first time, and second, subwavelength spatial resolution (12.6nm) imaging is achieved, also for the first time. The key to bothadvances is a novel technique, termed modulus enforced probe (MEP), which uses the far-field
diffraction of the illumination as a constraint in the CDI algorithm. This new technique enables
faster convergence, quantitative reconstructions, the ability to image periodic objects, and is robustin the presence of background noise. This work is important for high-resolution imaging of a broad
range of next-generation nanoscale electronics. 1

8.1

Introduction
High resolution imaging is needed to support the development of next-generation EUV lithog-

raphy, nanoelectronics, data storage, and self-assembled nanostructures, as well as functional imaging of nano-enhanced devices. Due to the wavelength dependent diffraction limit, short wavelength
1This chapter is adapted from Gardner et al. [173]55sources in the extreme-ultraviolet (EUV) and soft X-ray regions of the spectrum are attractive forhigh resolution imaging. However, most EUV optics are costly, imperfect, lossy, and cannot reachdiffraction-limited spatial resolution. Coherent diffractive imaging (CDI) techniques, as discussed
in chapter 6, address the critical limitations in EUV optics by employing computational techniques
to form images. Moreover, CDI techniques are the most photon efficient form of imaging because
there are no lossy optics between the sample and the detector [117]. Using CDI, it is now possible
to achieve diffraction-limited spatial resolution at short wavelengths.
For non-periodic samples, the CDI technique known as ptychography (Sec. 6.3) can reliably,and simultaneously, solve for the sample and illumination. On the other hand, periodic samples posea particular challenge to CDI techniques because the lack of diversity in the diffraction patterns,
resulting in poor convergence of the algorithm [125, 130, 140, 163, 174, 175]. Moreover, the spatial
resolution achieved to date, for real-world objects under good reconstruction conditions, was limited
to 1.3× the wavelength (λ) [168].
In this work, using a tabletop 13.5 nm high harmonic light source, a sub-wavelength resolution (0.9λ) image of an extended sample is achieved in the EUV region for the first time. Also for
the first time, high-fidelity, full-field, quantitative imaging of near-periodic objects is demonstrated
with CDI. The key to achieving high-fidelity images of periodic samples is a novel constraint termed
Modulus Enforced Probe (MEP). The new constraint, MEP, is based on one additional measurement of the illumination on the detector. This additional measurement is then used within aptychography algorithm, such as the extended ptychographic iterative engine [150], to highly constrain the guess for the illumination beam. Furthermore, the measurement of the illumination isa measurement of the total power of the input beam allowing quantitative amplitude and phase
information for both the sample and illumination. Using the MEP technique also improves therobustness of the algorithm in the presence of noise, reduces artifacts from cross-talk between thesample and illumination, and converges in fewer iterations. To my knowledge, the experimental
demonstration discussed in this thesis, is the best resolution-to-wavelength ratio for any full-field,
non-isolated sample, CDI-based microscope.

56

8.2

Experimental set-up and Modulus Enforced Probe methodology
Bright, phase-matched, high harmonic beams (see Ch. 4) are generated in a KMLabs eX-

treme Ultraviolet Ultrafast Source by focusing an ultrafast infrared driving-laser into a helium-filled
waveguide. The driving-laser is a 3 kHz KMLabs Dragon centered at a wavelength of 785 nm, with
23 fs pulse duration and 2 mJ pulse energy. The laser is focused and coupled into a 150 µm diameter waveguide, filled with 500 Torr of helium, which is carefully engineered to minimize thereabsorption of the EUV radiation. After the high harmonic generation in the waveguide, mostof the residual infrared light is removed by a beam separator: a Brewster-angle silicon substratecoated with ≈210 nm of ZrO2 [137, 176–178]. Any residual infrared light after the beam separator
is removed with a 600-nm thick zirconium filter.
As shown in Fig. 8.1, a pair of Si/Mo multilayer mirrors are used to select and focus a single
harmonic order, at a wavelength (λ) of 13.5 nm ± 0.2 nm, onto the sample. The angle of incidence
on the mirrors is estimated to be 2◦ ± 0.5◦ from normal, with a 100 mm radius of curvature on thesecond mirror. Using a knife-edge measurement at the sample plane, the EUV focus is measured
to be 2 µm ± 0.5 µm in diameter. A scanning electron microscope (SEM) image of sample isshown in the inset of Fig. 8.1. The sample, placed at the focus and perpendicular to the EUV
beam, is a zone plate with 150 nm-thick polymethylmethacrylate (PMMA) rings on a 50 nm silicon
nitride window. The sample was scanned in an 11 × 11 rectilinear pattern with nominally 0.88
µm between adjacent positions. A random offset of ±20% of the step size is added to each scan
position to prevent periodic artifacts from being introduced by the scan grid itself [154]. At eachscan position, the EUV light scattered by the sample is detected on back-illuminated chargedcoupled device (Andor iKon) with an array of 2048 x 2048 square 13.5 µm pixels placed 22.6 mm± 0.2 mm from the sample. Each recorded diffraction pattern is two accumulations at 4.25 second
exposure time, with 2×2 binning on-chip, at a 1 MHz pixel readout rate. After collection, and after
the on-chip binning, the diffraction patterns were cropped to 900 × 900 pixels. A representative
diffraction pattern, including stray HHG light that bypassed the multilayer mirrors, is shown in

57
Fig. 8.1. The sample was scanned in the top-right quadrant, such that the strongest diffracted
light scattered along the diagonal of the detector, thereby maximizing the numerical aperture (NA)of the microscope. The scattered light was detected at an NA of 0.54 corresponding to an Abbe
diffraction limited resolution, ∆r, given by Eq. 8.1, where λ is the wavelength, and NA is thenumerical aperture.

∆r =λ= 12.5 nm ± 0.2 nm
2 NA

(8.1)

There are many ways to employ the novel modulus enforced probe (MEP) methodology. In
the first method, depicted in Fig. 8.2, the sample is moved out of the EUV beam path, and a single
image of the direct illumination is collected under the same, or similar, experimental conditions
as the ptychographic dataset. The collection of the direct, un-scattered beam, can be carried out
before or after the acquisition of the ptychographic dataset. In a reflection geometry, rather than
the transmission geometry presented in this work, a measurement of the specular reflection off ofa smooth surface can be used as the un-diffracted beam. Unlike the transmission geometry, where
no information about the sample is needed for quantitative imaging, in a reflection geometry thereflectance of the surface is needed to scale the beam data for quantitative imaging. However, it
is possible and has recently been demonstrated for quantiative analysis of buired layers [179]. The
data for the MEP constraint can be obtained by separating the DC (zero-order diffraction) fromthe rest of the scatter pattern. This last method is especially effective when the sample is too large
to be removed from the beam path or the ptychographic dataset has already been acquired and nomeasurement of the direct beam was taken. The third approach is used in this demonstration anddiscussed in detail in the following section.

8.3

Intensity assignment to the extracted zero-order diffraction peak
While removing the sample and collecting the direct beam is the most straight forward of

the MEP methodologies (Fig. 8.2), a measurement of the raw beam without the sample was

58

Figure 8.1: Modulus enforced probe coherent EUV microscopy A 13.5 nm harmonic beam
is selected and focused, using a pair of multilayer mirrors, onto a zone plate sample. The sample
is raster scanned and the scattered EUV is collected on a charged-coupled device (CCD) at anumerical aperture, NA, of 0.54. In addition to scattered light from the sample, some backgroundlight is also recorded on the CCD. The inset shows a scanning electron microscope (SEM) imageof the sample’s upper right quadrant, where the EUV data was collected.

59
not taken under the same experimental conditions as the ptychographic dataset in this work. It
was only during post-processing that a new constraint was discovered to improve convergence andimage quality. To apply the MEP constraint without the collection of the un-scattered beam,
the zero order, or DC component, of the diffraction patterns must be extracted from the dataset.
Furthermore, for quantitative imaging the correct intensity must be assigned to the isolated DC
peak.
The un-diffracted beam is extracted using a three step process. First, to wash-out sample
dependent features, the mean of the ptychographic dataset is computed. Then the diffraction
peaks are isolated by thresholding at 30% of the maximum value. And finally, the DC peak is
spatially isolated from the other peaks. The isolation of the DC peak is not necessary in the caseof weakly scattering objects. With weakly scattering objects, the DC peak may be extracted byonly thresholding. In experiments with photon flux that may cause damage to the detector, suchas x-ray sources at free-electron laser facilities, weakly scattering objects can be used to attenuate
the beam.
After extracting the DC peak, the correct intensity must be assigned to for quantitative
imaging. If the average transmission of the sample is known, this information may be used to scale
the DC peak. Alternatively, if the flux of the input beam is known, this information can also be
used to scale the DC peak. The latter technique is used in this work.
The flux of our HHG beam is frequently monitored by recording the maximum count on thesame detector used for data collection without any samples in the beam path. The camera setting
for the max count measurement had the following settings: 2 × 2 binning, one accumulation, 0.1
second exposure, and 3 MHz readout rate. This resulted in a maximum count value of 23,550
after subtracting the offset from the camera’s analogy-to-digital converter. The maximum count in
extracted DC peak was scaled to match the maximum count of our flux measurement after adjustingfor differences in camera settings. After adjusting the max count for differences in exposure timeand accumulations, the max count assigned to the DC peak is 2, 119, 500. The extracted and scaled
DC peak is shown in Fig. 8.2 as if it were collected with the sample removed.

60

Figure 8.2: Modulus enforced probe methodology The modulus enforced probe constraint
uses the direct beam as a constraint in the ptychography algorithm. One strategy to obtain theun-scattered beam is to move the sample out of the beam path, either immediately before or after
the ptychographic data collection, and record the direct beam. Another strategy is to isolate thezero order weak from the collect ptychographic data set. The latter is employed here and the zeroorder peak is depicted on the detector.

61

8.4

Sub-wavelength coherent imaging of extended near-periodic objects
After collection of the ptychographic dataset and the extraction of the zero-order diffraction

as the MEP constraint, intensity images are reconstructed using the ePIE algorithm [150] with andwithout the MEP modification. Sub-regions of reconstructed intensity images of the zone plate aredisplayed in Fig. 8.3, with the full reconstruction displayed in Appendix D. As a reference for image
quality, a scanning electron microscope (SEM) image is shown in Fig. 8.3a. The reconstructed
image with the MEP constraint, Fig. 8.3b, is of much better quality than the image without the
MEP constraint, Fig. 8.3c, and compares favorably with the SEM image in the same region. The
inverted contrast between the SEM image and the ptychographic images is a result of the different
imaging geometries; the SEM image was taken in a reflection geometry and the ptychography data
was obtained in a transmission geometry.
Imaging periodic samples represents a major challenge in traditional ptychographic CDI, due
to the lack of diversity in the diffraction patterns, resulting in poor convergence and artifacts.
Although the width of the PMMA zone plate rings have a radial dependence proportional to 1/r,
with r = 40µm being the radius of the outer-most ring, the rings within the 5.65µm × 5.65µm area,
shown in Fig. 8.3, constitute a quasi-periodic arrangement of lines. When the MEP methodology
is not applied, Fig. 8.3c, artifacts, as indicated by stripes and rapid oscillations, are present in theimage. On the other hand, with application of the MEP constraint, Fig. 8.3b, the artifacts areeither removed or reduced.
The insets of Fig. 8.3, show the periodic arrangement of 8 PMMA lines with 110 nm ± 10nm width spaced by 90 nm ± 10 nm of Si3 N4 . To determine if the reconstruction resolution isconsistent with the numerical aperture (NA) of the collected diffraction patterns, a lineout acrossa zone plate PMMA feature is analyzed with and without the MEP constraint. The location of thelineouts are shown by the lines inside the insets of Fig. 8.3b,c. The profile of the PMMA featuresare shown in Fig. 8.4a. The profile with MEP is shown by blue circle data points and was fitted
to an error function. The 10% - 90% width of the fit (r-square better than 0.97) is approximately

62
6 nm and is better than our reconstruction pixel size, dx, given bydx =λz= 12.6 nm ± 0.2 nm
N px

(8.2)

where λ is the wavelength, z is the distance from the CCD to the sample, N is the number of pixels
on the detector, and px is the effective pixel size with on-chip binning. The agreement between the12.5 nm Abbe limit from the numerical aperture (NA) of the collected diffraction patterns and the12.6 nm resolution supported by the lineout of the zone plate feature, with the MEP constraint,
substantiates that the algorithm was able to converge to a solution limited only by the NA of thedata, and demonstrates sub-wavelength EUV imaging for the first time.
Due to the presence of artifacts in the image without the MEP constraint, 10 parallel andadjacent profiles were averaged for the lineout analysis. The orange square data points in Fig. 8.4acorrespond to the lineout without MEP. The lineout is fitted to an error function (r-squared better
than 0.98) and the 10% - 90% values of the fit support a 60nm resolution.
In addition to the sub-wavelength resolution of 0.9λ with the MEP constraint, we can also
obtain three-dimensional topographical information from the phase image as shown in Fig. 8.4b.
To create the topographic image from the phase (shown in Appendix D), the phase informationmust be converted to a physical thickness. The intensity image of the zone plate, inset of Fig.
8.3b, is used to create two binary masks: a mask for the PMMA features and a mask for the
Si3 N4 substrate. To separate the two materials, a threshold of 1/3 of the theoretical transmissionof Si3 N4 [180] is used to separate the materials. The phase of the Si3 N4 was fitted to a 2nd orderplane, using a non-linearly least squares routine, and the fitted phase plane was subtracted from theentire phase image. Phase values below −π are wrapped around to lie between −π and π. Within
the PMMA features, values less than 3× the standard deviation of the substrate were increasedby π to unwrap the phase. With the flattened and unwrapped phases, the thickness is calculatedusing the reported index-of-refraction values of PMMA for 13.5nm radiation [180]. The resulting
3D image is interpolated onto a 4× larger grid and the vertical scale is scaled by 1/5. The height ofthe zone plate features are calculated to be 180 nm ± 40 nm.

63Figure 8.3: Record sub-wavelength resolution imaging using 13.5 nm light and Modulus
Enforced Probe a) Scanning Electron Microscope (SEM) image of the zone plate sample. b)
Intensity image from the ptychographic reconstruction, in the same region as the SEM image,obtained with the novel Modulus Enforced Probe constraint. The use of the MEP constraint
results in quantitative transmission values of the sample. c) Ptychographic reconstruction without
the MEP constraint results in degraded reconstruction quality and unphysical transmission values.
Due to the contrast mechanisms of the SEM in a reflection geometry, the contrast of the SEM
image is inverted with respect to ptychographic images obtained in a transmission geometry. The
insets show a zoomed in region of the image and the lines within the inset indicate the location of
the knife edge test, shown in Fig. 8.4.

Figure 8.4: Zone plate PMMA feature lineout and topographic image a) The lineouts of a
PMMA feature along the lines shown in the insets of Fig. 8.3a,b. The blue and orange data points,
with error-function fits (solid lines), correspond the images with and without the MEP constraint.
The distance between the 10% - 90% values of the MEP constrained lineout fit supports subwavelength resolution at 12.6 nm . b) Topographic image obtained by converting the phase image,with the MEP constraint, to height using the PMMA index-of-refraction. The vertical scale bar
has been scaled by 1/5 and the image has been interpolated unto a 4× larger grid. The blue planeshows the location of the lineout in (a).

64
An important implication of the MEP constraint is quantitative imaging as shown in Fig.
8.3b. Quantitative reconstructions allow for materials to be identified and has been used to investigate oxide formation in buried structures [179]. Without the MEP constraint, power in thealgorithm is allowed to flow between the object and probe, which can lead to unphysical transmission values as seen in Fig. 8.3c. The average transmission value of the 50 nm thick Si3 N4 region(bright areas in the inset of Fig. 8.3b) is 0.44 ± 0.2. This transmission value is lower than thetabulated value, 0.65, reported in Ref. [180]. The difference may be explained by the incomplete
liftoff of the PMMA, as can be seen in the SEM images of the sample shown in Fig. 8.1 and Fig.
8.3a.
The discrepancy between the tabulated and reconstruction values of the 150 nm thick PMMA
regions (dark areas in the inset of Fig. 8.3b) are larger than the Si3 N4 discrepancy. The tabulated
value of PMMA is 0.46 [180] compared to 0.05 ± 0.04 in the reconstructed image. While thereconstructed transmission of PMMA is inconsistent with the tabulated value, the reconstructedvalue is consistent with a transmission measurement of the zone plate using the same setup for theptychographic data collection. The transmission measurement was performed near the central diskof the zone plate and not the upper-right quadrant where the ptychography scan was performed.
The mismatch in transmission values was noticed only after the data collection, otherwise thetransmission measurement would have been in the same location as the ptychography scan.
The transmission measurement was performed as follows. Keeping all the detector settings
the same, a diffraction pattern is collected with and without the zone plate in the beam. The
transmission of the zone plate, after the subtraction of detector readout noise, is the sum of thediffraction with the zone plate divided by the sum of the diffraction without the zone plate. The
calculation of the transmission, including both the PMMA and Si3 N4 , yielded a value of 10.9%. To
determine the transmission of PMMA, the SEM image, shown in Fig. 8.1, is used to determine thearea occupied by PMMA vs. Si3 N4 near the central disk. The result of the PMMA transmission
calculation is 0.05 ± 0.03, with the uncertainties coming from the threshold value used to separate
PMMA and Si3 N4 in the SEM image, uncertainties in the beam size, and uncertainties in the

65location of the measurement. Further exploration of the low transmission of PMMA is beyond thescope of this work, but possible reasons include the sample‘s age and its storage. The sample waspurchased in 2004, was stored in atmosphere, exposed to room lights, and contaminated with dust
because it was not stored in a clean room environment. To summarize, the transmission values
obtained with the MEP methodology, in contrast to unphysical values obtained without MEP, arereasonable and consistent with experimental transmission measurements.
The MEP constraint enables unique capabilities for periodic object reconstructions by minimizing the cross-talk between object and probe. The minimization of cross-talk, or decoupling
between the probe and sample reconstructions, are seen by comparing the reconstructed probes
shown in Fig. 8.5. The reconstructed probe with the MEP constraint (Fig. 8.5a,b) is smoothand continuous, while without the constraint (Fig. 8.5c,d) the probe is of poor quality. The poor
quality probe leads to a poor quality sample reconstruction because the ptychography algorithm’sreconstruction of the sample is dependent on the probe (and visa-versa). The lack of diversity inthe diffraction patterns from periodic objects means less information for the algorithm, and maylead to poor decoupling of the object and probe, as seen in this work. Therefore, additional information introduced by the MEP constraint is especially important in reconstructing the probe fromperiodic samples.
The additional information from the MEP constraint leads to quantitative reconstructions
because the MEP constraint eliminates the transfer of power between the sample and the illumination. In ptychography without the constraint, the power of the exit-surface wave, or product of
the sample and illumination, is fixed by the power in the measured diffraction. As a result, poweris able to flow, inside the algorithm, between probe and sample because the product is unaffected,
leading to unphysical transmission values as seen in Fig. 8.3c. The MEP constraint eliminates
this transfer of power, because the power of the probe is enforced in addition to the diffraction
measurement. Therefore, the reconstructions of the sample and illumination are quantitative (Fig.
8.3b).
With the exception of the MEP constraint, the reconstructions procedure is identical. The

66

Figure 8.5: Minimization of cross-talk with the modulus enforced probe constraint a)
The intensity and b) the phase of the 13.5 nm illumination (probe) at the sample plane with the
Modulus Enforced Probe (MEP) constraint. The probe is smooth and continuous and is in contrast
to c) the intensity and d) the phase of the illumination without MEP. Without the MEP constraint,
there is cross-talk, or poor decoupling, between the illumination and sample reconstruction, Fig.
8.3c, leading to artifacts and degraded image quality. The probe intensity is shown in detector
counts and the scale bar in (a) applies to all the panels.

67
Table 8.1: Reconstruction parameters

Stage 1
Stage 2
Stage 3
Stage 4

Total Iterations
950
700
10,00010,000Probe Updates
100-950
100-700
2000-9000
2000-9000

Position CorrectionNoNoNo
2-9000reconstruction was done in four stages using the ePIE ptychography algorithm [150] on a Nvidia
GPU (Tesla k-40). The initial probe guess for the algorithm was generated by modelling the opticalcomponents in the beamline; the initial object guess was unity. In the first two stages a binary
mask was used to block the stray background light during the modulus constraint; the modulus
constraint was not applied in the background region, instead the values were set to zero.
Table 8.1 summarizes the parameters of the four reconstruction stages. After completion of
the first stage, the updated probe was used as the initial probe guess for stage two; the object
was re-initialized to unity. Stage three began in the same manner as stage two, with the updated
probe from the end of stage two as the initial probe guess and the object re-initialized to unity.
In stage three, principles discussed in Ref. [181] were used to let the algorithm fill in data in themasked-off background region. In other words, the modulus constraint was not enforced in the straybackground region and the algorithm filled in these regions. Finally, in stage four, both the probe
and object at the end of stage 3 are used as the initial guesses. As in stage 3, the algorithm wasallowed to extrapolate values in the background region. During this last stage, position correction,
as described in Ref. [170], was performed. The reconstruction as the end of stage four are shownin Fig. 8.3, Fig. D.1, and Fig. D.2.

8.5

Implementation of the Modulus Enforced Probe Constraint
The ptychography algorithm, as described in sec. 6.3, solves for both the object and the probefrom a set of diffraction measurements. With one additional measurement of the un-diffracted
illumination, a powerful constraint is possible. This novel constraint is termed Modulus Enforced

68
Probe (MEP) and the general working principle is displayed in Fig. 8.6.
It is assumed the probe does not change during the scan. If the sample is removed fromthe beam path, either immediately before or after the ptychographic data collection, a direct
measurement of the probe, Pj (~u), can be recorded on the detector, which is given by
Pj (~u) = |F[P (~r − rj )]2 |.

(8.3)

Following the notation in 6.3.2 and 6.3.3, ~u is the spatial frequency vector at the detector plane, F
is the propagator from the sample to detector plane, ~r is the spatial coordinate vector at the sample
plane, rj is the shift for position j, P is the amplitdue of the probe at the sample plane, and P is
the intensity of the probe at the detector plane. The MEP constraint utilizes the measured probe
on the detector, Pj (~u), to constrain the guess of the probe in the ptychography algorithm. Whilethe implementation of MEP has not been investigated in all versions of ptychography, for example
see [149, 154, 156–158], here it is implemented as a modification to the ePIE algorithm [150]. The
constraint is introduced after the probe update function given by Eq. 6.13 in 6.3.3 . The updated
probe, PGj+1 (~r), is propagated to the detector plane forming a guess of the probe on the detector
given by, PGj (u) = F[PGj+1 (~r)]. Here, we apply a modulus constraint to the probe guess enforcing
the measurement
PM j (~u) =q

Pj (~u)PGj (u)|PGj (u|(8.4)

This modulus constrained probe guess, PM j (~u), is propagated back to the sample plane forming afurther updated probe guess0PGj+1(~r) = F−1 [PM j (~u)]

(8.5)

0
which is consistent with the measured probe at the detector. The new probe guess, PGj+1(~r), isnow fed back into the algorithm. This additional constraint to the probe is analogous to the errorreduction (ER) algorithm as described in by Fienup [119], but instead of using ER to solve for theobject, it is used within the ptychography algorithm to further constrain the probe guess. In thiswork, a simple version to enforce the probe measurement is used, but more advanced algorithms

69

Figure 8.6: Modulus Enforced Probe implementation within ptychography algorithm
The updated probe from the ptychography algorithm is further constrained with measurement of
the un-diffracted probe. First, the update probe is propagated to the far field. In the far field, theamplitude is replaced with the measured amplitude. Then the probe is inverse transformed backto the sample plane and feedback into the ptychography algorithm. This sequence of steps is themodulus enforced probe implementation with the ptychography algorithm.

70such as hybrid input-output [120], or relaxed averaged alternating reflections (RAAR) [134] can be
used.

8.6

Modulus Enforced Probe Simulations
In this section, the effects of the MEP constraint on convergence, initial probe guesses, andnoise are explored using simulated data. The simulation parameters are given in Table 8.2 andwere chosen to follow the experimental conditions. The complex-valued sample, for the simulation,
was composed of open-source test images2 ; the amplitude and the phase are shown in Fig. 8.7a
and Fig. 8.7b, respectively. The simulated probe, also shown in Fig. 8.7a,b, consists of a Gaussian
profile with a 1/e width (σ) equal to 2µm. The probe has a hard edge at r = 2µm and one Fresnel
zone of phase curvature. The 7 × 7 scan positions, with r/3 step size, are shown as green dots on
the amplitude of the sample (Fig. 8.7a), with the total reconstruction area outlined in green. The
simulation uses the ePIE algorithm as described in Ref. [150]. There is no sub-pixel shifting, instead
the shift is rounded to the nearest pixel. The alpha and beta feedback parameters are unity. The
scan positions are called in the same order for each iteration. To propagate between the sample
and detector, a normalized fast Fourier transform (FFT) is used [166, 167].
In the first simulated reconstruction, the initial guess of the probe is the probe used tosimulate the ptychographic dataset; the initial object guess is unity. Three tests are performed: noprobe updates, as well as probe updates with and without the MEP constraint. The results of thesimulation are shown in Fig. 8.8 and Table 8.3. In Fig. 8.8 a plot of the root-mean-square (RMS)
is shown, where the RMS error defined byqP
RM S =Xjn (|Ψj (u)| −p

Ij (u))2

M ×N

(8.6)

where Ψj (u) is the FFT of the exit surface wave, Ij (u) is the intensity of the diffraction patternon the detector, M and N are the dimensions of the grid, and j is the index of the scan position.
Table 8.3 shows the total time of the simulation and the number of iterations to reach convergence.
2

https://commons.wikimedia.org/wiki/Main_Page Tv resolution chart and Ishihara Test

71
Table 8.2: Modulus Enforced Probe Simulation Parameters
Wavelength
λ = 13.5 nm
CCD pixel(no bin)px = 13.5 µm

Sample-to-CCD
z = 22.6 mm
Binning
2×2

Probe Radius
R = 2 µm

Scan Size
7×7

Step Size
R/3

Gaussian Widthσ = 2µ m

Number of Pixels (no bin)
256 × 256

Probe Update
iteration 10

The times of the simulation can be greatly improved by using GPU computing, as done in theexperimental results above. However for these simulation, the reconstructions were done on asingle Intel CORE i5 CPU.
The reconstruction converges in fewer iterations with the MEP constraint, but the additional
FFTs needed for the MEP constraint result in a longer per iteration time. The combination of
fewer iterations to converge and a longer per iteration time nearly balance out; it took 2% longer,
it time, to converge with the MEP constraint than without it. In future work, the MEP constraint
does not need to be applied at each iteration nor each position of each iteration. Instead, the MEP
constraint could be applied to some subset of the iterations or scan positions. Further simulations
are needed to find the balance between convergence in fewer iterations and faster iterations times.
Furthermore, the feedback parameter on the probe udpates, β [150], can be increased with the MEP
constraint as discussed in the simulation sections of [173], and leads to even faster convergence.
The next test uses random initial probe guesses cropped to three radii: r = 1µm, 2µm, and3µm. Both the amplitude and phase of the initial probe guesses are random with the amplitude
values between 0 and 1 and the phase values between −π and π. The results of this simulation
are shown in appendix D.3. With the MEP constraint the algorithm still converges, even with therandom guesses of the probe. This suggests that as long as the diffraction patterns are properly
sampled, no knowledge of the probe is needed at the sample plane with the MEP constraint; thefar-field information of the probe is sufficient for the algorithm to converge. On the other hand,
without the MEP constraint, the algorithm will not converge with random guesses.
The effects of additive white Gaussian noise are also investigated. The addition of white

72

Figure 8.7: Ptychography with MEP: simulated sample a) The amplitude and b) phase of thecomplex-valued simulated sample. The green dots on shown in (a) indicate the scan positions used
to simulate the ptychographic dataset. The green outline shows the area scanned by the probes.
The insets in (a) and (b) show the simulated probes amplitude and phase.

Figure 8.8: Perfect Initial Probe Guess Simulated Reconstruction In this test, the initialprobe guess is the probe used to generate the simulated data. The plot shows the root-mean-squareerror of the reconstruction as a function of iteration. The algorithm converges faster with the MEP
constraint than without it.

73
Table 8.3: Few iterations to converge with MEP
Total
Total Time per Iterations to Time to
Iterations Time(s) Iteration(s) Converge Converge(s)No Probe Updates
600
165
0.275
372
102
Probe Updates
600
193
0.322
583
188
Probe Updates w/ MEP
600
246
0.410
469
192

Gaussian noise reduces the ratio of signal to noise ratio (SNR) and two SNR values were simulated:
100 dB and 50 dB. The noise was added to the simulated diffraction patterns. In both cases, theptychography algorithm with the MEP constraint reached a lower RMS error than without the
MEP constraint as shown in appendix Fig. D.4. The MEP constrained algorithm reached 83% and
85% better RMS error for the 100 dB and 50 dB SNR simulations.

8.7

Conclusion
By applying the novel modulus enforced probe technique (MEP), a spatial resolution of

0.9 × λ was demonstrated on an extended, quasi-periodic object using 13.5 nm illumination.
Without the MEP constraint, the resolution is lower, 60 nm, and suffers from cross-talk between
the object and the probe leading to a poor quality image. With the MEP constraint, the achieved
12.6 nm ± 0.2 nm spatial resolution is in agreement with the theoretical Abbe resolution of 12.5 nm± 0.2 nm corresponding to the numerical aperture. To my knowledge, this is a record resolutionto-wavelength ratio for any EUV or x-ray full-field image of an extended object. Moreover, thiswork is the first high-quality image of a periodic sample using a coherent diffractive imaging.
Ongoing research in ptychography, including imaging with multiple colors [182–184], undersampling [185, 186], and thick samples [187–190], will all benefit from the from the MEP constraint
because the addition information introduced. In these ongoing efforts, the algorithm is tasked withsolving form more than just a single sample and illumination, thus the additional information from
the MEP constraint reduces the number of unknowns in the algorithm.
As the techniques presented here are scalable, illumination with shorter wavelengths, eitherwith tabletop high-harmonic sources or large-scale synchrotrons and x-ray free electron lasers, can74
enable nanometer, or even atomic scale resolution, of a broad range of next-generation electronics
such as semiconducting chips and data storage devices.

Chapter 9

Stroboscopic Imaging of Thermal Transport in Nanostructures

The fastest processes at the nanoscale, such as heat transport [191], shock waves in plasma[192], and ultrafast magnetization [193, 194], happen at the picosecond (ps) to femtosecond (fs)time scales. Optical pulses have made it possible to temporal resolve dynamics at these timescales,
but the spatial resolution of these wavelengths are not sufficient to image the nano scale features
directly. Thus, to capture the fast dynamics and image the features simultaneous pulses of shortwavelengths are employed [195].
Ultrafast electron microscopes have been developed [23, 24] an can achieve nanometer scalespatial resolution, with 100 fs temporal resolution. The ability to obtain shorter pulses mainly
limited by space-charge effects and is an active area of research [25]. Complementary to ultrafast
electron microscopes are pulsed sources of coherent EUV and X-rays. Without imaging, shortpulses of x-rays were used to analysis the Airy diffractions of circular samples using model based
approaches [196,197]. Extreme ultraviolet lasers have been used, with their nanosecond (ns) pulses,
to image an oscillating magnetic nano probe using Fresnel Zone plates [198] and, with Fouriertransform holography, imaged a vibrating cantilever. Coherent diffractive imaging techniques havebeen employed ultrafast imaging of samples in a single shot [199, 200].
In this chapter, we explore stroboscopic imaging of micron to nanoscale structures using
high-harmonic generation sources. As discussed in Ch. 4, the radiation from HHG maintains the
temporal structure of the driving laser and is inherently synchronized in time with the IR driving
laser making HHG the ideal source for tabletop pump-probe experiments. The IR light is used to76thermal excite the sample and the EUV, in combination with ptychographic coherent diffractive
imaging (CDI), is used to image the sample with and without the excitation of the pump. The
analysis of the images shows a 3 Å axial expansion of the sample when excited with the pump.

9.1

Pump-Probe Principles
In pump-probe experiments, the sample is excited with the pump and measured with theprobe. It is critical that the pump pulses are synchronized with the probe pulses with little jitter
between the pulses. Typically, this is accomplished by splitting a pulsed laser into a pump-arm
and a probe-arm. The relative path length of each arm can be adjusted, enabling control over thearrival time of the pump and probe pulses. If the sample dynamics are reversible, then stroboscopic
imaging is possible by taking snap shots of the sample at various pump-probe delays.
The timing of pump-probe pulses can be divided into three categories: positive time, timezero, and negative times. These different pumping schemes are depicted in Fig. 9.1. Positive timerefers to instances where the pump beam reaches the sample before the probe. This allows the
sample to be excited before the measurement by the probe. The simultaneous arrival of the pumpand the probe is called time zero. At this instant, the beams are overlapped in time and the sample
begins to be respond to the pump. Negative time occurs when the probe arrives before the pump.
During negative time, the probe does not measure the pump‘s excitation of the sample.

9.2

Experimental Geometry
The temporal resolution of the this stroboscopic imaging system is on the order of femtosec-

onds, and is limited by the pulse length of our driving laser (21-24 fs). The timing between pulses
is 200 µs, or 5kHz repetition rate, and is long enough to ensure the sample dynamics have relaxed
before arrival of the next pump pulse [191].
Before the generation of harmonics, but after the beam stabilization mirrors, part of thedriving laser is split off into a separate beam path called the pump-arm. The pump-arm is depicted
in Fig. 9.2. It is critical that the pump-arm be split off after beam stabilization mirrors because

77

Figure 9.1: Pump-Probe Timing In a pump-probe experiment, the pump pulse excites the
sample and then a probe pulse measures the excitation (positive-time). The simultaneous arrivalof the pulses is time zero. When the pump arrives after the probe, the probe does not measure theexcitation by the pump pulse (negative-time).

78
if not, the beam stability feedback will introduce spatial beam jitter or walk off. The driving laser
is separated with a 70:30 beam splitter with low dispersion characteristics. The reflected beam issent towards the high-harmonic waveguide (not shown in Fig. 9.2), while the transmitted beam
travels through a half-wave plate and polarizer combination allowing for tunable pump fluence andpolarization. The delay stage consists of two components: an Areotech ANT130 motorized linear
stage with nanometer precision and a retro-reflecting mirror. The retro-reflector is carefully design
to reflect the beam parallel to the input beam, but shifted laterally. The total distance of thepump-arm was designed to equal that of the probe arm when the delay stage is nearly at the end of
its negative-time range. This alignment enables investigation farther into the positive time regime,
allowing for more dynamics of the samples to be captured.
Before the pump beam enters the experimental chamber, through a sapphire window, afocusing lens is placed on a linear, micrometer-actuated, stage. The lens focuses the pump beam
onto the sample plane. The stage allow the lens to be moved along the optical axis enabling finecontrol of the spot size on the sample which was fine tuned to ≈350 µm diameter. At the mostnegative-time delay position of the stage, the spot size is 385µm x 304µm. While at the other endof the stage, the most positive-time, the spot size is 393µm x 309µm. The change is spot size isdue to slight misalignment of the delay stage, which causes the beam to point differently throughthe focusing lens. The sample is placed before the focal spot and the spot size is measured using a
CMOS detector (Mightex S-series). After the lens, the pump beam is steered into the experimental
chamber with an ultra-stable tunable mirror mount. This adjustable mirror mount enables fineadjustments of the pump beam, without altering the alignment through the focusing lens.
In the following experiments, the pump beam is the driving laser (780nm) and the probe
beam is the high-harmonic radiation (≈30nm) (Fig. 9.1). The pump beam is used to heat the
sample before the arrival of the probe. The probe scatters off the sample and is recorded on a
detector as depicted in Fig. 9.3. The camera used in the experiment is a Princeton Instruments
in-vacuum camera with a back-thinned CCD. The CCD has a square array of 2048x2048 pixels,
each with a side length of 13.5µm. The entire camera and readout electronics are placed inside

79

Figure 9.2: Pump-Probe Schematic After the beam stabilizing mirrors, the driving laser is split
into two paths. One path, the probe arm, is steered towards the HHG waveguide. The other path,
the pump-arm, is steered into a delay stage. Movement of the delay stage alters the path length
enabling control of the pump-probe timing. A λ/2 wave plate and polarizer combination are used
to adjust the pump fluence. A lens outside the experimental chamber focuses the pump onto thesample. The path length of the pump-arm is carefully designed to match the length of the probe
arm and is not drawn to scale here.

80
the evacuated experimental chamber. Feedthroughs for electrical and cooling were installed. The
chiller, used to pump a 50:50 mixture of distilled water and propylene glycol, was customized forlow vibration pumping.
The pump beam at least 105 to 106 times brighter than the high-harmonic radiation, thus thecamera will completely saturate or become damaged if the pump light reaches the CCD. To protect
the CCD, and only measure the scattered EUV light, a 200nm thin aluminum filter, was installedover the CCD. The filter holder was designed to mount directly over the CCD and contained
a baffling system for safe evacuation and venting of the chamber. As determined by recording
a negligible increase in CCD background counts with a pump power of 1 W, the pump light is
attenuated by at least 10−6 .
To ensure synchronization of the pump and probe pulses with the camera exposure, two
in-vacuum shutters are adopted. In addition to these shutters, a third shutter is installed, labeled
the “alternating shutter” in Fig. 9.3. This shutter is physical located outside by chamber, but isdepicted inside for simplicity. The alternating shutter, as the name suggests, opens every-otherexposure. Thus, when the data are collected there is a pump-on exposure, followed by a pump-off
exposure. This is important during data analysis because the pump-off data acts as a control set.
Changes from pumping should only be present in the pump-on exposure. Changes in the pump-off
signal indicate some changes in the HHG beam or irreversible sample changes, such as melting or
burning.
Before the ellipsoidal mirror shown in Fig. 6.3, a single harmonic from the HHG comb isselected using a pair of 45 degree angle-of-incidence SiC/Mg multilayer mirrors. The distance fromexit of the waveguide to the center of the ellipse is 1500mm and the ellipse to focus distance is
100 mm. The sample is placed at the focus of the ellipse with a 3-axis stage. The HHG beam isincident on the sample at an angle of 62 degrees from the sample normal (28 degrees glancing) with
the CCD placed 47.5mm from the sample and perpendicular to the specular reflection.

81

Figure 9.3: The pump-probe experimental chamber The HHG beam is focused onto thesample with an ellipsoidal mirror. The sample scatters EUV light onto the in-vacuum detector.
The detector has a 200nm aluminum filter in front of the CCD to block the pump light. A shutter
is used to alternatively block the pump; there is one measurement with excitation from the pump,followed by a measurement without excitation.

82

9.3

Experimental characterization of the Time-resolved ptychographic CDI
microscope
The stroboscopic EUV microscope presented in this thesis is the first of its kind. Therefore,

after its development, a series of tests was required to ensure its correct implementation. The
verification of time zero is first done outside of vacuum with a Beta Barium Borate (BBO) crystal,a common nonlinear optical material, using the IR laser instead of the HHG radiation. Withsufficient intensity, 150-300 mW, the IR light from the driving laser can frequency double inside
the crystal. If two ultrafast beams are overlapped on the BBO crystal, non-collinearly, in both timeand space, an additional cross-correlation signal is generated [201]. The cross-correlation signal is
only present at time zero. Without generating high-harmonics, some of the driving light is passed
through the probe arm, into the chamber, and off the ellipsoidal mirror. The sample, as shown in
Fig. 9.3, is replaced with the BBO crystal. Finding the autocorrelation signal from the BBO in
this manner, provides an estimate of the delay stage location corresponding to time zero.
After this step, a more precise estimate of time zero needs to be determined in vacuum,
overlapping spatially and temporally the the HHG radiation from the probe path with the IRpump beam. To accomplish this, the spatial overlap in the chamber in vacuum condition is first
determined with an external imaging system which consists of mirrors placed inside the chamber
to relay light reflected off the sample out through a transparent viewport and into a telescopic lenssystem mounted on a CMOS detector. A LED white light is attached to a viewport on the chamber
to illuminate the sample. The aluminum filter, mentioned in the previous section, mounted on the
CCD blocks the white light from the LED, allowing real-time monitoring of the sample during datacollection.
To visualize the HHG beam on the sample plane, a featureless area of the sample is coatedwith a thin layer of phosphorus. When the phosphorus is illuminated with HHG, it fluoresces inthe visible spectrum which is detectable with the external imaging system. The pump light isalso visible on the phosphorus, thus allowing the visualization of the overlap pump and probe in83vacuum, at the sample plane.
In vacuum, as discussed thus far, only the spatial overlap of the pump and probe beam havebeen accomplished. The next step is verifying temporal overlap. Verification of temporal overlap
is achieved by detecting a time-dependent change in scatter from a calibration sample consisting aperiodic array of lines, 500nm in width with a 75% duty cycle, composed of 8nm tall nickel features
patterned on silicon. This sample scatters light into distinct orders as seen by a representative
diffraction pattern shown in Fig. 9.4a.
The thermal response of this sample was reported in Ref. [191], where the dynamics occurredon the order of picoseconds. The dynamics of this sample include longitudinal acoustic waves (LAW)
and surface acoustic waves (SAW). The LAW waves are the vibrations of the nanostructures after
the rapid thermal expansion from the pump pulse. The SAW waves are acoustic modes that are
confined to a very shallow penetration depths [202] and have been used to characterize the nanoscale
properties such as the mechanical properties of thin films [203].
As the grating-like sample is rapidly heated by the pump beam, thermal expansion from thegrating lunches LAW and SAW waves, which cause the relative height of the lines to change withrespect to the substrate. The changing height of the grating causes a phase shift of the scattered
light resulting in a change in the diffraction efficiency of the grating at the detector plane. Thechange is diffraction is quantified bychange in dif f raction =(AC + + AC − ) − DC
AC + + AC − + DC

(9.1)

where AC + and AC − are the total power in the positive and negative first order diffraction peaks,
and DC is the zero order peak. The peak regions used for the calculation are shown in Fig. 9.4a.
This type of analysis have been employed previously to investigate the dynamics of surface acoustic
waves and nanoscale heat transport [191, 202, 203].
In this work, the change in diffraction signal is used to verify the presence of a dynamic signal
and is shown as a function of pump-probe delay in Fig. 9.4b. The figure shows the signal with andwithout the pump accomplished by switching of the alternating shutter (Fig. 9.3). The relatively

84

Figure 9.4: Verifying time zero with a grating sample a) Scattered EUV from a Ni grating
sample. The grating sample scatters the EUV into distinct orders. The orders highlight with theboxes were used in the change in diffraction calculation, Eq. 9.1. b) The change in grating efficiencychanges when the grating is heated by the pump light. The abrupt change in diffraction indicatesthe location of time zero.

85
flat pump-off signal compared to the pump-on, Fig. 9.4b, indicates the change in diffraction is dueto heat expansion of the grating and not fluctuations in the HHG source. The abrupt jump in thepump-on signal is the location of time zero. The change in diffraction signal ensures that the pumpand probe beams are overlapped in both space and time. Furthermore, the signal-to-noise ratio issimilar to previously published work [191, 202], and both the LAW and SAW waves are visualized.
The LAW waves are the rapid oscillations in the pump signal, see Fig. 9.4b, immedialty following
time zero. The SAW wave is the longer period wave, and with our delay stage range, just over afull period was captured. With a more range, the SAW wave exponentially deceares and the heatfrom the sample disipates [202].

9.4

Dynamics from a gold circuit-like sample
The detailed characterization of the stroboscopic EUV microscope enbaled the investigationof the thermal response from a gold circuit-like sample, by means of time-resolved ptychographic
CDI. The sample was fabricated using e-beam lithography on a silicon substrate and consists of 29
nm tall features of evaporated gold on a 5 nm titanium adhesion layer. 1
A static ptychography scan is taken on the gold circuit sample. To prevent periodic artifacts[154], while maintaining uniform overlap of the sample, the scan follows a Fermat spiral trajectory[155]. The step size between positions is 2µm with a total of 197 positions. At each scan position,
3 accumulations, at 1 second exposure time, are acquired with 2x2 binning on chip. The static
ptychography reconstruction is shown in Fig. 9.5. Figure 9.5a is the amplitude and Fig. 9.5b is
the phase. In the upcoming experiments, when the sample is pumped, a phase change is expected
because the pump will heat up the sample causing thermal expansion. The expansion of thefeatures, relative to the substrate, results in a phase shift to larger values.
Using the same principles to verify alignment of the pump and probe on the grating sample,
diffraction patterns are collected from the gold sample as a function of pump-probe delay. First, thestage is moved to its most negative-time position and a total of 50 diffraction patterns were collected1

sample fabricated at JILA by Christina L. Porter

86

Figure 9.5: Static Gold Circuit Reconstruction The a) amplitude and b) phase of the gold
circuit sample reconstructed from a static ptychography scan.

87

Figure 9.6: Dynamic Signal from Circuit Diffraction a) An example of the diffraction fromthe circuit sample with the beam at the center of the features. The boxes highlight the zero andfirst order peaks. b) Using the change in diffraction equation, Eq. 9.1, and the highlighted regionsin the diffraction, a pump-probe signal is extracted.

(25 pump-on and 25 pump-off). The collection of at least 50 negative-time diffraction patterns isdone to allow the sample to thermalize and reach thermal equilibrium. After thermalization, thestage is moved in 2ps steps until it reached its positive-time limit. Including pump-off and pumpon exposures, a total of 780 diffraction patterns were collected, with a representative diffraction
pattern is shown in Fig. 9.6a, to generate the time trace shown in Fig. 9.6b.
Each collected diffraction pattern has an exposure time of 0.4 seconds with 2 x 2 binningon-chip and 2 accumulations. To speed up the data acquisition, only a subset of the detector was
read-out in the vertical direction: 832 vertical x 2048 horizontal pixels (before binning). The input
pump-power was measured at 76.2mW. The spot size of the pump, 350µm, was measured at the
sample plane with a CMOS detector at the 1/e2 intensity.
The diffraction in Fig. 9.6a does show first order peaks, but it is not as pronounced as thegrating sample diffraction (Fig. 9.4a) due to the non-periodicity of the sample. As a result, thechange-in-diffraction signal, Fig. 9.6b, is not as distinct as the signal from the grating, Fig. 9.4b, as
quantified by the small percent change in the signal. Nevertheless, the signal is present and verifies
the pump and probe are spatially and temporally overlapped on the gold circuit sample.
The static reconstruction in Fig. 9.5 and the pump-probe change in diffraction signal seen in

88Fig. 9.6b confirms the proper configuration of the experiment. In a stroboscopic fashion, images are
obtained using ptychography. In total, 4 ptychography scan are acquired: two scans at negative timewith the pump-on and pump-off, and two scans at positive time with the pump-on and pump-off.
At negative times, the probe scatters off the sample before the pump heats the sample. Therefore,
there should be no change in the phases at negative times. On the other hand, at positive-time thesample is heated by the pump before the arrival of the probe, thus a phase change in the pump-on
image with respect to the pump-off image is expected.
The pump-on and pump-off scan at negative time is intentional, even though theoretically thephases should be the same. The purpose of the pump-on/pump-off negative images is a measurement of the repeatability and stability of the microscope. In fact, if there are statistically significant
differences in the phases at negative time between pump-on/pump-off, then the microscope, in its
current form, is not suitable for detection of small phase shifts from nano to micron scale structures
because the signal is buried in the noise.
The parameters for each of the 4 stroboscopic ptychography scans are identical. Each scanconsisted of 122 scan positions in a Fermat spiral pattern with 2µm between adjacent positions.
The camera was set to readout out full-chip images at 1MHz readout rate with 2x2 binning on-chip
at 0.5 second exposures and 4 accumulations. A total of 488 diffraction patterns are collected overapproximately 1 hour and 40 minutes. A full ptychography scan is taken, then the alternating
shutter switches states i.e., a pump-off ptychographic data set is collected followed by the pump-on
ptychographic data set.
In addition to the recorded diffraction patterns, other measurements are taken and used fordata analysis, namely beam and background data. Before and after the ptychography scans at aparticular pump/probe delay, beam data is acquired by moving the features of the sample out of
the beam path, such that the beam reflects off the silicon substrate. This beam data is used as
the modulus enforced probe constraint as discussed in Sec. 8.5. The beam data, before and after
scans, also measures the beam drift and changes in intensity. Background data is taken with thegas removed from the high-harmonic waveguide and is used to characterize detector‘s readout noise

89
and hot pixels, as well as any stray light on the detector.
The phase images from the ptychography scans are shown in Fig. 9.7 and Fig. 9.8. Figure
9.7 shows the phases at the most negative-time delay position of the stage, with the pump-on (Fig.
9.7a) and the pump-off (Fig. 9.7b). The phases of these images are displayed in a histogram plot
in Fig. 9.7c with a bin width of 2π/200. Similarly, 9.8a and 9.8b show the pump-on and pumpoff phase images at the most positive-time delay position, with 9.8c showing the histogram phase
distribution.
The phase reconstructions shown in Fig. 9.7 and Fig. 9.8 followed an identical analysis
procedure. In the first step, the processing consisted of background subtraction and titled plane
correction [165, 168, 169]. After titled plane correction, the diffraction patterns were cropped to
512 x 512 pixels. The retrieved probe from the static reconstruction was used as an initial probe
guess. The initial object guess is always unity with no phase. The ptychographic reconstructions
were done in three stages. First, the ptychography algorithm with the modulus enforced probe
constraint ran for 200 iterations with probe updates allowed after iteration 11. After the firststage, the updated probe was cropped with a super Gaussian, order 60, with σ = 25 µm. The
cropped probe was fed back into the algorithm for stage two. Stage two consisted of 250 iterations
with probe updates after iteration 30. The modulus enforced probe constraint was only used in
the first stage and not in second or third stage. During stage two, the same super Gaussian used
to crop the probe was enforced during the probe updates. The enforcement of the super Gaussianeliminates noise from build-up at the edges of the updated probe. After the second stage, theretrieved probe was again cropped with a super Gaussian, order 60, but with σ = 15µm. The
cropped probe was fed into the algorithm for stage three. Stage three ran for 1000 iterations withno cropping of the probe. Position correction, as described by Ref. [170], was preformed between
iterations 50 and 500. Updates to the probe were allowed between iterations 501 and 900. While
the ptychography algorithm is a powerful phase retrieval algorithm, there are some ambiguities inreconstructions. There can be translations in the reconstructed images, which correspond to linear
phase shifts. There can also be an overall offset in the phase between reconstructions.

90

Figure 9.7: Negative Time Phase Distribution At negative time, the probe scatters off thesample before the pump. Therefore, there should be no difference in phase between pump on andpump off. The phase images a) with and b) without the pump. c) A histogram, π/200 bin width, ofthe phases (dots) with a double Gaussian best fit (solid line).The black bars at the bottom of thegold phase distribution guide the eye to the area used in t-test.

91

Figure 9.8: Positive Time Phase Distribution At positive time, the pump heats the sample
before the probe scatters off the sample. Therefore, a phase shift between pump on and pump off
from thermal expansion is expected. The phase images a) with and b) without the pump. c) A
histogram, π/200 bin width, of the phases (dots) with a double Gaussian best fit (solid line).

92
Before we can compare the phases from the four reconstructions, the phase ambiguities need
to be addressed. With this aim, each reconstruction is aligned to each other, by whole-pixel
shifting, such that the gold features are in the same location. After aligning, the central region of
the reconstruction is cropped at 200 x 200 pixels. A preliminary phase shift compensation is doneby taking a histogram of the phase, with 2π/200 bin widths, and calculating the center-of-mass. The
center-of-mass of the phase distribution is set to zero. The shifting of the center-of-mass ensures
the peaks in the histogram from the substrate and gold phases fall around zero. Without shifting
the center-of-mass, the gold phase peak, for example, may be near +π and wrap around to −π.
The next step is using the phase histogram to separate the substrate from the gold features.
With the center-of-mass of the phase distribution set to zero, the histogram is fit with adouble Gaussian:f (χ) = a1 ∗ exp(−((χ − b1 )/c1 )2 ) + a2 ∗ exp(−((χ − b2 )/c2 )2 )(9.2)

where χ the location of the histogram bin center, a the amplitude, b the offset, c the width (or σ)of the Gaussian, with the subscripts denoting the first and second Gaussian parameters. The fit isdone by a non-linear least squares routine with the coefficient of determination (R2 ) better than
0.96 for all the fits. The minimum phase value between the two Gaussian fits is used to separate
the phase into two categories: the substrate and gold. The substrate region of the phase image is
fit to a 2nd order plane given by
P f it(x, y) = p00 + p10 × x + p01 × y + p20 × x2 + p11 × x × y + p02 × y 2(9.3)

where the pXX‘s are the coefficients of a 2nd order plane, with x and y the coordinates of thephase image. The fitted plane is subtracted from the entire phase image (both the gold andsubstrate). Subtracting the fitted plane removes any phase ambiguities from the reconstructions
due to phase shifts and offsets. The second order plane is used, instead of a first order, because
a quadratic phase may introduced from sample bending or an inaccurate sample-to-CCD distancemeasurement. Regardless of the cause of phase distortion in the image, subtracting the fitted phaseallows for a direct comparison of the phases from different reconstructions.

93
After flattening the phases by subtracting the 2nd order plane fit, the phase image is again
divided into a histogram and fit to a double Gaussian. The peak of the first Gaussian, the substratepeak, is shifted so the maximum counts is arbitrarily aligned to −pi/3. The alignment of all thesubstrate peaks to −pi/3 allows a direct comparison of the gold feature phase distributions as shownin Fig. 9.7c and Fig. 9.8c.

9.5

Statistical significance of the phase shifts
As shown in Fig. 9.7c, the pump-on and pump-off phases at negative-time appear to be

identical. On the other hand, the gold phase distribution shown in Fig. 9.8c shows a slight shift
with the pump-on as compared with pump-off. In order to determine if the phase shift from thepump at positive-time is statistically significant, a Welch’s t-test (or unequal variances t-test) is
performed. A t-test can determine if the means of two normal distributions are statistically different
and is given by
ttest =
with the degrees of freedom Ω,x̄2 − x̄1
σ12
σ2
( N1 + N22 )1/2
σ2

Ω=

(9.4)

σ2

( N11 + N22 )2
σ14
σ24
+
2
N1 ν1
N12 ν2(9.5)

where x̄ is the mean, σ is the standard deviation, N is the number of points, and ν = N − 1.
The subscripts 1 and 2 denote the pump-off and pump-on phases, respectively. The t-test assumes
normal distributions and from the Gaussian fits with R2 better than 0.96, that assumption isreasonable. Since the peak substrate phase has been assigned the value of −pi/3, only the gold
phase distribution is analyzed with the t-test. To separate the gold phase from the substratephase, the phase at the trough between the two fitted peaks, plus 0.24 radians, is used divide thedata (see black bars in Fig. 9.7c). Phases greater than the trough are considered the gold phase,as long as the counts are greater than the counts at the trough. Removing phase values with fewer
counts than the trough-point removes the tail of points extending to π. The black bars in Fig. 9.7c
guide-the-eye to the points selected for the t-test. The points selected for the t-test are shown in94

Figure 9.9: Statistical z-test on gold phase distributions The phase histogram distributions for(a) negative and (b) positive time. A t-test is used to determine if the means of these distributions
are statistically different.

Fig. 9.9.
The mean is calculated from the histogram distribution. Each point in histogram corresponds
to the number of pixels that fall within the bin width. The mean is the central bin value multipliedby the number of counts divided by the total number of counts,x̄ =counts × phase.
Σ counts(9.6)

The standard deviation is estimated the from difference between the max and min phasevalues of the gold phase distribution divided by six, because in a Gaussian distribution 96% of
the data falls within six standard deviations. A summary of the values used for the t-test aresummarized in table 9.1. The t-test results for the negative and positive times are 0.6 and 1.2,
respectively. Using a t-test significance look up table, and the given number of data points anddegrees of freedom, the negative time delay phase distributions are indistinguishable. On the other
hand, there is a marginal statistical difference between the pump-on and pump-off phase.

95
Table 9.1: Statistical significance determined with a t-testx̄ meanσ variance
N data points
Welch’s t-test
degrees of freedom
confidence level

9.6

Negative Timepump-on pump-off
1.274
1.248
0.17280.188537370.577672∼0%

Positive Timepump-on pump-off
1.204
1.152
0.17280.1883
34
36
1.242
68
∼75%

Calculation of the height change from thermal expansion
The change in height from thermal expansion is calculated using two methods. The first

method uses the difference in mean values between the gold phase distributions from the histogram(Fig. 9.9). The difference in the mean values, shown in Table 9.1, is 0.05 radians, and using thefollowing equations:
∆d =

∆φλ
2π

(9.7)

∆h =

∆d
2 cos θ(9.8)

the change in height ∆h is calculated, where ∆d is the optical path length difference, ∆φ is thephase change in radians, λ is the wavelength, and θ is the angle of incidence on the sample (fromnormal). This calculation yields a height change of 2.4 Å.
The other method uses the phase difference between the substrate and gold features tocalculate to the height of the gold. In order to compare the phase from the different materials, thephase change upon reflection needs to be calculated. The procedure used here is adapted from Ref.
[204], which describes how to calculate the complex reflection coefficient from a stack of materials.
The complex indices of refraction where taken from Ref. [180]. The thickness of the silicon oxide
layer, 3 nm, was measured on a similar substrate in previous work using ellipsometry [169]. Taking
into account the phase change upon reflection, the average phase change between the substrate
and the gold feature is 7.23 radians with the pump off and 7.29 radians with the pump on. Using96
equations 9.7 and 9.7, the heights of the gold features are 35.3 nm and 35.6 nm, respectively,
corresponding of a thermal expansion induced height change of 3 Å.

9.7

Summary and Future work
The design and implementation of an extreme ultraviolet microscope capable of stroboscopic

ultrafast temporal resolution is demonstrated here with a preliminary data analysis. Some of thenear-infrared driving laser is split-off before the high-harmonic generation and used to heat the
sample. Spatial and temporal alignment of the system was verified with a grating sample, using
similar techniques described previously [191,202,203]. The thermal expansion of the grating, due toheating from the pump, causes a time dependent change in diffraction. A non-periodic sample wasthen used and ptychographic scans were collected, with and without the pump, and negative andpositive time delays. The phase reconstructions demonstrate a 3 Åheight change at from thermal
expansion.
While there is a difference, between the pump-on and pump-off phase at positive times, thestatistical difference is marginal. Using the same data set, the statistics may improve with further
data processing. For example, letting the ptychography algorithm iterate for longer, i.e. 10,000
iterations instead of the 1450 used here, will allow the phase distribution to converge to a morehomogeneous value thereby strengthening the significance of the t-test. For reference, over 10,000
iterations were used to obtain the high-fidelity images with sub-wavelength resolution discussed in
the previous chapter (Ch. 8); therefore using the same number of iteration here is reasonable.
There are also many other datasets not presented here that show promising dynamics, suchas datasets in which a 16 µm diameter circular nickel structure was pumped. The reconstructionof this data set suggests a radial expansion of 100nm, with a 1nm axial expansion, when pumped.
The challenge with the circle data is the time trace analysis because the diffraction from the circle
does not of clear diffraction orders. New methods for detecting changes in diffraction are currently
being investigated, including radially averaging techniques.
To improve future data collections the camera readout time needs to be faster. As of right97
now, nearly all of the data collection time is readout. Typical exposures for the dynamic data sets
were less than a second, but it takes about 15 seconds to readout the CCD. With the ability toreadout faster, many more ptychography scans could be taken immediately following time zero andafter reconstruction and registering the images, a movie could be rendered.
The methodology described here can be used to study scientifically relevant samples in thenear future. For example, the techniques described here can be combined with newly demonstrated
circularly polarized high-harmonic generation [205, 206] for magnetic domain imaging [207, 208].
The combination of the pump and EUV probe tuned to a magnetic edge, can be used to study
ultrafast demagnetization [194], which is important for next-generation data storage devices.

Chapter 10

Conclusion

10.1

SummaryThis thesis discussed methods for high-resolution static and stroboscopic microscopy using

tabletop coherent extreme ultraviolet (EUV) light from tabletop high-harmonic generation (HHG)
sources (Ch. 4). An ultrafast Ti:Sapphire laser was up-converted using HHG to either 30 nm or 13.5
nm harmonics, depending on the demonstration. The coherent short wavelength sources were combined with a lensless, computational, phase and amplitude-contrast technique called ptychographic
Coherent Diffractive Imaging (CDI) (Ch. 6).
In this work, a combination of experimental methods for high-numerical aperture data collection and novel computational algorithms enabled the highest resolution-to-wavelength imaging
using CDI and EUV in both reflection and transmission geometries. For ptychographic CDI imaging
in a reflection geometry, the titled plane correction algorithm [165] was developed, which enabled
high-resolution imaging of surfaces in a reflection geometry (Ch. 7). An EUV microscope with 40
nm transverse resolution and 6 Åaxial resolution using 30 nm radiation was developed [168].
A powerful technique termed modulus enforced probe, was developed in this work whichenables both imaging of periodic objects and convergence of the ptychographic CDI algorithm infewer iterations (Ch. 8). The novel constraint consists of on additional measurement of the unscattered illumination at the detector plane, which is used to tightly constrain the algorithms guessof the illumination. The MEP constraint was used to achieve a record subwavelength resolution
image, 12.6 nm, of an extend periodic sample in the EUV spectral region using the technologically

99
relevant wavelength of 13.5 nm [173].
Furthermore, the ultrafast pulse durations in the femtosecond (fs) range of the high-harmonicsource were harnessed to demonstrate proof-of-principle pump-probe imaging of nanostructures(Ch. 9). Some of the IR light used to generate the harmonics, was split off and used to pumpa sample with micron to nanoscale structures. Two images of the structure were taken stroboscopically, and captured the thermal excitation of the nano-features with an axial resolution of 3
angstroms (Å).

10.2

Future WorkIn Ch. 7, high numerical aperture CDI imaging was demonstrated in a reflection geometry

for the first time. The structures used for the EUV demonstration (Sec. 7.2) had low, on theorder of one, aspect ratios: the ratio of feature depth to wavelength-of-illumination. Some workon high aspect ratio structures has been done in a transmission geometry [209], but thus far there
have been no reflection demonstrations in the EUV or x-ray spectral regions. The ability to image
high-aspect ratio structures further opens up the applicability of EUV CDI.
Regarding the Modulus Enforced Probe (MEP) constraint discussed in Ch. 8, further simulations and demonstrations are needed. With simulated data, it was seen that the ptychographyalgorithm converges in fewer iterations with MEP, but the iteration time per iteration is slower.
With a modified application of MEP, such that it is only applied every five or ten iterations, it issuspected that the convergence properties will be nearly the same, but the per iteration time will
be much faster. Simulations and experimental demonstration of CDI on a near-perfect periodic
sample will be exciting future work. Of particular importance, is the imaging of self-assembled
periodic structures from block copolymers [210]. These structures are promising as the building
blocks of nano-engineered systems, but are sometimes difficult to image using electron microscopies
because they are non-conducting, low-z, materials.
Many opportunities remain to be explored with the newly demonstrated EUV dynamic imaging capabilities. In the immediate future, there needs to be more data processing of acquired data,

100
especially of data acquired on a 16 µm nickel disc sample and on a 750 nm nickel grating. In
preliminary analysis, the nickel disc sample shows about a 100nm radial and 1nm axial thermal
expansion due to pumping. The grating sample is also promising, but reconstruction quality is poorat the moment. Application of the MEP constraint and more iterations may yield better images.
The development of a new algorithm is needed to verify a time-dependent change in diffraction
signal due to pumping. As discussed in section 9.3, the diffraction peaks of a grating were used
to verify the spatial and temporal alignment of the pump and probe. This is a powerful tool andhas been used to study nanoscale heat flow [191, 202, 203], and a similar techniques have analyzed
the Airy diffraction patterns from circular samples [196, 197]. In its current form, this techniqueonly work for periodic objects, or simply circular shapes, with well-known diffraction. For a general
structure, it does not perform well. An algorithm capable of quantify changes in diffraction patterns
from general structures, but is insensitive to fluctuation in high-harmonic radiation, is needed toopen up the EUV stroboscopic microscope to a broader sample set.
In future stroboscopic EUV microscope systems, a camera with faster readout is critical. The
largest bottle neck in data collection is the readout of the CCD. The exposure time is less than asecond, even with multiple accumulations, but the readout time takes 15 seconds or longer. The
recently released, commercially available, back-illuminated CMOS cameras will enable faster datacollection, so more snapshots of the sample can be taken enabling movies showing the angstromscale axial dynamics of nanoscale features.

10.3

Future Outlook
One of the advantages of EUV and x-ray wavelengths is the long penetration depths comparedwith electron microcopy methods, allowing for the imaging of buried surfaces non-destructively. A
recent demonstration used EUV at 30 nm to image below an optical opaque film of aluminum (seeFig. 10.1). [179]. Currently under development are experimental methods and algorithms to image
the interior of objects, without the need to physically slice the sample. Instead, these techniques
computationally decompose the sample into thin slices, tasking the ptychography algorithm to solve

101for each slice, such that the resulting exit-surface-wave, when propagated to the detector plane, isconsistent with the measurement [187–190]. These three-dimensional algorithms are likely to beadapted to image high-aspect ratio structures in a reflection geometry.

Figure 10.1: EUV imaging through metal A planarized damascene sample, copper and silicon,
is coated with 100nm Al. The aluminum coating prevents an optical microscope from imaging theburied surface. With EUV, the damascene sample is imaged with and with the metal coating.
Figure adapted from Ref. [179].

The analysis of the phase distribution in the stroboscopic images, section 9.4 and 9.5, suggest
3 angstrom resolution in the axial direction. In future work, an analytical expression for the phaseresolution is of interest. The ability to image atomic layers should be possible and can be tested oncleaved SiC wafers used for atomic force microscopy calibration. These sample are nearly-periodic,
but the application of the MEP constraint should enable reconstructions.
Typically, a single harmonic is used for imaging, but recent work has shown simultaneous
illumination of a sample with multiple harmonics (see Fig. 10.2a) [211]. The ptychography algorithm then reconstructs an image for each harmonic. In the future, this methodology can beapplied with harmonics spanning atomic edges providing elemental contrast without the need toscan wavelengths with hardware.

102
In related work, it has been shown that different areas of the sample can be imagined simultaneously, with different probes, allowing larger fields of view with a single scan [212]. In the same
work, it was also shown that orthogonal polarization states can be used in image a sample simultaneously (see Fig. 10.2b). Employing polarization sensitivity in the EUV, in combination with
CDI, will allow for a complete characterization of how light interacts with the sample: amplitude,
phase, and polarization contrast.
An exciting possibility is tabletop magnetic imaging using the newly demonstrated circularly
polarized high-harmonics (see Fig. 10.2c) [205, 206, 213]. The circularly harmonics, if properly
tuned to the magnetic edge, can be used to image magnetic domains, as done at large scale facilities[98, 208, 214].
All of the techniques developed in this thesis are scalable to shorter wavelengths, wavelengths
shorter than a nanometer using mid-IR driving lasers (see Fig. 10.2d) [63,84,85]. Furthermore, thestroboscopic methods discussed can employ short pulses, pulses as short as attoseconds [30,89]. The
combination of attosecond pulses with soft-x-ray HHG, will probe the fastest dynamic processes at
the nanoscale.

103

Figure 10.2: Possibilities for future work a) EUV hyperspectral imaging with simultaneous
illumination of harmonics. In the future, harmonics spanning atomic transitions can be used forelement specific imaging. Panel adapted from Ref. [215]. b) Polarization multiplexed ptychography
can be applied in the EUV for a complete characterization of lights interaction with the sample.
Panel adapted from Ref. [212] c) The generation of circularly polarized HHG can be used to image
magnetic samples. Panel adapted from Ref. [206] d) The generation of sub-nanometer soft-x-ray
from mid-IR driving lasers will lead to higher spatial and temporal EUV microscopy. Panel adaptedfrom Ref [63]Bibliography[1] R. Hooke, Micrographia, or Some physiological descriptions of minute bodies (J. Martyn and
J. Allestry, London, 1665), 1st ed.
[2] D. Evanko, A. Heinrichs, and C. K. Rosenthal, “Milestones in Optical Microscopy,” Nat. Cell
Biol. 11, S56 (2009).
[3] “Numerical aperture of a thin lens by Moxfyre at English Wikipedia [Public domain], via
Wikimedia Commons,” .
[4] J. Squier and M. Müller, “High resolution nonlinear microscopy: A review of sources andmethods for achieving optimal imaging,” Rev. Sci. Instrum. 72, 2855–2867 (2001).
[5] W. R. Zipfel, R. M. Williams, and W. W. Webb, “Nonlinear magic: multiphoton microscopy
in the biosciences.” Nat. Biotechnol. 21, 1369–77 (2003).
[6] J.-X. Cheng and X. S. Xie, “Coherent Anti-Stokes Raman Scattering Microscopy: Instrumentation, Theory, and Applications,” J. Phys. Chem. B 108, 827 (2004).
[7] U. Dürig, D. W. Pohl, and F. Rohner, “Near-field optical-scanning microscopy,” J. Appl.
Phys. 59, 3318–3327 (1986).
[8] E. Betzig, A. Lewis, A. Harootunian, M. Isaacson, and E. Kratschmer, “Near Field Scanning
Optical Microscopy (NSOM),” Biophys. J. 49, 269–279 (1986).
[9] E. H. Synge, “XXXVIII. A suggested method for extending microscopic resolution into theultra-microscopic region,” London, Edinburgh, Dublin Philos. Mag. J. Sci. 6, 356–362 (1928).
[10] E. A. Ash and G. Nicholls, “Super-resolution Aperture Scanning Microscope,” Nature 237,
510–512 (1972).
[11] A. Bek, R. Vogelgesang, and K. Kern, “Apertureless scanning near field optical microscopewith sub-10 nm resolution,” Rev. Sci. Instrum. 77, 43703 (2006).
[12] Z. Li, S. Yue, J. Chen, and Q. Gong, “Ultrafast spatiotemporal relaxation dynamics of excitedelectrons in a metal nanostructure detected by femtosecond-SNOM.” Opt. Express 18, 14232–
14237 (2010).
[13] T. A. Klar, S. Jakobs, M. Dyba, A. Egner, and S. W. Hell, “Fluorescence microscopy withdiffraction resolution barrier broken by stimulated emission.” Proc. Natl. Acad. Sci. U. S. A.
97, 8206–8210 (2000).

105[14] T. A. Klar, E. Engel, and S. W. Hell, “Breaking Abbe’s diffraction resolution limit in fluorescence microscopy with stimulated emission depletion beams of various shapes.” Phys. Rev.
64, 066613 (2001).
[15] R. M. Dickson, a. B. Cubitt, R. Y. Tsien, and W. E. Moerner, “On/off blinking and switching
behaviour of single molecules of green fluorescent protein.” Nature 388, 355–358 (1997).
[16] R. Henriques, C. Griffiths, E. H. Rego, and M. M. Mhlanga, “PALM and STORM: Unlocking
live-cell super-resolution,” Biopolymers 95, 322–331 (2011).
[17] E. Betzig, G. H. Patterson, R. Sougrat, O. W. Lindwasser, S. Olenych, J. S. Bonifacino,
M. W. Davidson, J. Lippincott-Schwartz, and H. F. Hess, “Imaging intracellular fluorescentproteins at nanometer resolution.” Science 313, 1642–5 (2006).
[18] L. de Broglie, “Recherches sur la théorie des quanta (Researches on the quantum theory),”Ann. Phys. 3 (1925).
[19] E. Ruska and M. Knoll, “Die magnetische Sammelspule für schnelle Elektronenstrahlen. (Themagnetic concentrating coil for fast electron beams.),” Z. Tech. Phys. 12, 389–400 (1931).
[20] M. M. Freundlich, “Origin of the Electron Microscope,” Science 142, 185–188 (1963).
[21] A. Bogner, P. H. Jouneau, G. Thollet, D. Basset, and C. Gauthier, “A history of scanningelectron microscopy developments: Towards ”wet-STEM” imaging,” Micron 38, 390–401(2007).
[22] K. W. Urban, “Is science prepared for atomic-resolution electron microscopy?” Nat. Mater.
8, 260–2 (2009).
[23] B. Barwick, H. S. Park, O.-H. Kwon, J. S. Baskin, and A. H. Zewail, “4D Imaging of Transient
Structures and Morphologies in Ultrafast Electron Microscopy,” Science 322, 1227 – 1231
(2008).
[24] A. H. Zewail, “Four-Dimensional Electron Microscopy,” Science 328, 187–193 (2010).
[25] T. Van Oudheusden, P. L. E. M. Pasmans, S. B. Van Der Geer, M. J. De Loos, M. J. Van
Der Wiel, and O. J. Luiten, “Compression of subrelativistic space-charge-dominated electron
bunches for single-shot femtosecond electron diffraction,” Phys. Rev. Lett. 105, 1–4 (2010).
[26] G. Binnig and H. Rohrer, “Scanning Tunneling Microscopy,” IBM J. Res. Dev. 44, 279 (1993).
[27] G. Binnig, C. F. Quate, and C. Gerber, “Atomic Force Microscope,” Phys. Rev. Lett. 56,
930–933 (1986).
[28] S. Weiss, D. F. Ogletree, D. Botkin, M. Salmeron, and D. S. Chemla, “Ultrafast scanningprobe microscopy,” Appl. Phys. Lett. 63, 2567–2569 (1993).
[29] N. Khusnatdinov, T. Nagle, and G. Nunes, “Ultrafast scanning tunneling microscopy with 1
nm resolution,” Appl. Phys. Lett. 77, 4434–4436 (2000).
[30] T. Popmintchev, M.-C. Chen, P. Arpin, M. M. Murnane, and H. C. Kapteyn, “The attosecond
nonlinear optics of bright coherent X-ray generation,” Nat. Photonics 4, 822–832 (2010).

106[31] “Adiagramoftheelectromagnetic
spectrum,showingvariousproperties across the range of frequencies and wavelengths by Inductiveload,
NASA
[GFDL
(\url{http://www.gnu.org/copyleft/fdl.html)
or
CC-BY-SA-3.0(http://creativecommons.org/licenses/by-sa/3.0/},” .
[32] D. H. Bilderback, P. Elleaume, and E. Weckert, “Review of third and next generation synchrotron light sources,” J. Phys. B At. Mol. Opt. Phys. 38, S773–S797 (2005).
[33] T. K. Sham and M. L. Rivers, “A brief overview of synchrotron radiation,” Rev. Mineral.
Geochemistry 49, 117–147 (2002).
[34] J. D. Jackson, Classical Electrodynamics (Wiley & Sons, Hoboken, 1999), 3rd ed.
[35] D. J. Griffiths, Introduction to Electrodynamics (Prentice Hall, Upper Saddle River, 1999),
3rd ed.
[36] K. Willie, The Physics of Particle Accelerators, an Introduction (Oxford University Press,
Oxford, 2000).
[37] D. Attwood, Soft X-Rays And Extreme Ultravioet Radiation Principles and Applications(Cambridge, New York, 1999).
[38] A. Zholents and M. Zolotorev, “Femtosecond X-Ray Pulses of Synchrotron Radiation,” Phys.
Rev. Lett. 76, 912–915 (1996).
[39] R. W. Schoenlein, S. Chattopadhyay, H. H. W. Chong, T. E. Glover, P. A. Heimann, C. V.
Shank, A. A. Zholents, and M. S. Zolotorev, “Generation of Femtosecond Pulses of Synchrotron Radiation,” Science 287, 2237–2240 (2000).
[40] T. C. Marshall, Free-Electron Lasers (Macmillan Publishing Co., New York, 1985).
[41] C. Brau, “Free-electron lasers,” Science 239, 1115–21 (1988).
[42] C. A. Brau, Free-Electron Lasers (Academic Press, Inc., San Diego, 1990).
[43] H. P. Freund and T. M. Antonsen-Jr., Principles of Free-Electron Lasers (Springer, New York,
1992).
[44] E. L. Saldin, E. Schneidmiller, and M. V. Yurkov, The Physics of Free Electron Lasers(Springer, Heidelberg, 2000).
[45] P. Schmuser, M. Dohlus, and J. Rossbach, Ultraviolet and Soft-Ray Free-Electron Lasers(Springer, Heidelberg, 2008).
[46] B. W. J. McNeil and N. R. Thompson, “X-ray free-electron lasers,” Nat. Photonics 4, 814–821(2010).
[47] H. Motz, “Applications of the radiation from fast electron beams,” J. Appl. Phys. 22, 527–535(1951).
[48] H. Motz, W. Thon, and R. N. Whitehurst, “Experiments on radiation by fast electron beams,”
J. Appl. Phys. 24, 826–833 (1953).

107[49] J. M. J. Madey, “Stimulated emission of bremsstrahlung in a periodic magnetic field,” J.
Appl. Phys. 42, 1906–1913 (1971).
[50] L. R. Elias, W. M. Fairbank, J. M. J. Madey, H. A. Schwettman, and T. I. Smith, “Observationof stimulated emission of radiation by relativistic electrons in a spatially periodic transverse
magnetic field,” Phys. Rev. Lett. 36, 717–720 (1976).
[51] D. A. G. Deacon, L. R. Elias, J. M. J. Madey, G. J. Ramian, H. A. Schwettman, and T. I.
Smith, “First Operation of a Free-Electron Laser,” Phys. Rev. Lett. 38, 892–894 (1977).
[52] P. Emma, R. Akre, J. Arthur, R. Bionta, C. Bostedt, J. Bozek, a. Brachmann, P. Bucksbaum, R. Coffee, F.-J. Decker, Y. Ding, D. Dowell, S. Edstrom, a. Fisher, J. Frisch, S. Gilevich, J. Hastings, G. Hays, P. Hering, Z. Huang, R. Iverson, H. Loos, M. Messerschmidt,
a. Miahnahri, S. Moeller, H.-D. Nuhn, G. Pile, D. Ratner, J. Rzepiela, D. Schultz, T. Smith,P. Stefan, H. Tompkins, J. Turner, J. Welch, W. White, J. Wu, G. Yocky, and J. Galayda,“First lasing and operation of an ångstrom-wavelength free-electron laser,” Nat. Photonics
4, 641–647 (2010).
[53] S. Roling and M. Wöstmann, “The free electron laser FLASH,” (2015).
[54] D. L. Matthews, P. L. Hagelstein, M. D. Rosen, M. J. Eckart, N. M. Ceglio, A. U. Hazi,
H. Medecki, B. J. MacGowan, J. E. Trebes, B. L. Whitten, E. M. Campbell, C. W. Hatcher,A. M. Hawryluk, R. L. Kauffman, L. D. Pleasance, G. Rambach, J. H. Scofield, G. Stone,
and T. A. Weaver, “Demonstration of a soft x-ray amplifier,” Phys. Rev. Lett. 54, 110–113(1985).
[55] J. J. Rocca, “Table-top soft x-ray lasers,” Rev. Sci. Instrum. 70, 3799 (1999).
[56] J. J. Rocca, V. Shlyaptsev, F. G. Tomasel, O. D. Cortzar, D. Hartshorn, and J. L. A. Chilla,“Demonstration of a discharge pumped table-top soft-x-ray laser,” Phys. Rev. Lett. 73, 2192–
2195 (1994).
[57] S. Heinbuch, M. Grisham, D. Martz, and J. J. Rocca, “Demonstration of a desk-top size highrepetition rate soft x-ray laser.” Opt. Express 13, 4050–4055 (2005).
[58] D. Alessi, Y. Wang, B. M. Luther, L. Yin, D. H. Martz, M. R. Woolston, Y. Liu, M. Berrill,
and J. J. Rocca, “Efficient Excitation of Gain-Saturated Sub-9-nm-Wavelength Tabletop SoftX-Ray Lasers and Lasing Down to 7.36 nm,” Phys. Rev. X 1, 1–6 (2011).
[59] J. Bokor, P. H. Bucksbaum, and R. R. Freeman, “Generation of 355-nm coherent radiation,”Opt. Lett. 8, 217 (1983).
[60] A. McPherson, G. Gibson, H. Jara, U. Johann, T. S. Luk, I. a. McIntyre, K. Boyer, andC. K. Rhodes, “Studies of multiphoton production of vacuum-ultraviolet radiation in therare gases,” J. Opt. Soc. Am. B 4, 595 (1987).
[61] P. B. Corkum, “Plasma perspective on strong field multiphoton ionization,” Phys. Rev. Lett.
71, 1994–1997 (1993).
[62] M. Lewenstein, P. Balcou, M. Y. Ivanov, A. L’Huillier, and P. B. Corkum, “Theory of highharmonic generation by low-frequency laser fields,” Phys. Rev. A 49, 2117–2132 (1994).

108[63] T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O. D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth,A. Gaeta, C. Hernández-Garcı́a, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and
H. C. Kapteyn, “Bright coherent ultrahigh harmonics in the keV x-ray regime from midinfrared femtosecond lasers,” Science 336, 1287–91 (2012).
[64] J. Seres, E. Seres, A. J. Verhoef, G. Tempea, C. Streli, P. Wobrauschek, V. Yakovlev,
A. Scrinzi, C. Spielmann, and F. Krausz, “Laser technology: Source of coherent kiloelectronvolt X-rays,” Nature 443, 596 (2005).
[65] D. E. Spence, P. N. Kean, and W. Sibbett, “60-fsec pulse generation from a self-mode-locked
Ti:sapphire laser.” Opt. Lett. 16, 42–44 (1991).
[66] A. L. Lytle, “Phase Matching and Coherence of High-Order Harmonic Generation in Hollow
Waveguides,” Ph.D. thesis, University of Colorado (2001).
[67] J. Zhou, I. P. Christov, G. Taft, C.-P. Huang, M. M. Murnane, and H. C. Kapteyn, “Pulse
evolution in a broad-bandwidth Ti:sapphire laser,” Opt. Lett. 19, 1149–1151 (1994).
[68] M. Pessot, P. Maine, and G. Mourou, “1000 Times Expansion/Compression of Optical Pulses
for Chirped Pulse Amplification,” Opt. Commun. 62, 419–421 (1987).
[69] P. Maine, D. Strickland, P. Bado, M. Pessot, and G. Mourou, “Generation of Ultrahigh PeakPower Pulses By Chirped Pulse Amplification.” IEEE J. Quantum Electron. 24, 398–403(1988).
[70] D. Müller, S. Backus, K. Read, M. Murnane, and H. Kapteyn, “Very high-peakpower lasers:
cryogenic cooling multiplies ti:sapphire output,” Laser Focus World 41, 1–6 (2005).
[71] D. Strickland and G. Mourou, “Compression of amplified chirped optical pulses,” Opt. Commun. 56, 219–221 (1985).
[72] S. Backus, C. G. Durfee, M. M. Murnane, and H. C. Kapteyn, “High power ultrafast lasers,”
Rev. Sci. Instrum. 69, 1207–1223 (1998).
[73] S. Backus, R. Bartels, S. Thompson, R. Dollinger, H. C. Kapteyn, and M. M. Murnane,“High-efficiency, single-stage 7-kHz high-average-power ultrafast laser system,” Opt. Lett.
26, 465–467 (2001).
[74] M. D. Seaberg, “Nanoscale EUV Microscopy on a Tabletop: A General Transmission and
Reflection Mode Microscope Based on Coherent Di ractive Imaging with High Harmonic
Illumination,” Ph.D. thesis, University of Colorado (2014).
[75] H. C. Kapteyn, M. M. Murnane, and I. P. Christov, “Extreme nonlinear optics: Coherent X
rays from lasers,” Phys. Today 58, 39–44 (2005).
[76] G. Ndabashimiye, S. Ghimire, M. Wu, D. A. Browne, K. J. Schafer, M. B. Gaarde, and D. A.
Reis, “Solid-state harmonics beyond the atomic limit,” Nature 534, 520–523 (2016).
[77] U. Teubner and P. Gibbon, “High-order harmonics from laser-irradiated plasma surfaces,”
Rev. Mod. Phys. 81, 445–479 (2009).

109[78] J. Zhou, J. Peatross, M. Murnane, H. Kapteyn, and I. Christov, “Enhanced High-Harmonic
Generation Using 25 fs Laser Pulses,” Phys. Rev. Lett. 76, 752–755 (1996).
[79] Z. Chang, A. Rundquist, H. Wang, M. Murnane, and H. Kapteyn, “Generation of Coherent
Soft X Rays at 2.7 nm Using High Harmonics,” Phys. Rev. Lett. 79, 2967–2970 (1997).
[80] C. Durfee, A. Rundquist, S. Backus, C. Herne, M. Murnane, and H. Kapteyn, “Phase Matching of High-Order Harmonics in Hollow Waveguides,” Phys. Rev. Lett. 83, 2187–2190 (1999).
[81] A. Rundquist, C. G. Durfee III, Z. Chang, C. Herne, S. Backus, M. M. Murnane, and H. C.
Kapteyn, “Phase-Matched Generation of Coherent Soft X-rays,” Science 280, 1412–1415(1998).
[82] R. A. Bartels, A. Paul, H. Green, H. C. Kapteyn, M. M. Murnane, S. Backus, I. P. Christov,Y. Liu, D. Attwood, and C. Jacobsen, “Generation of Spatially Coherent Light at Extreme
Ultraviolet Wavelengths,” Science 297, 376–378 (2002).
[83] A. Paul, E. a. Gibson, X. Zhang, A. Lytle, T. Popmintchev, X. Zhou, M. M. Murnane, I. P.
Christov, and H. C. Kapteyn, “Phase-matching techniques for coherent soft X-ray generation,” IEEE J. Quantum Electron. 42, 14–26 (2006).
[84] M. C. Chen, P. Arpin, T. Popmintchev, M. Gerrity, B. Zhang, M. Seaberg, D. Popmintchev,
M. M. Murnane, and H. C. Kapteyn, “Bright, coherent, ultrafast soft x-ray harmonics spanning the water window from a tabletop light source,” Phys. Rev. Lett. 105, 1–4 (2010).
[85] C. Ding, W. Xiong, T. Fan, D. D. Hickstein, T. Popmintchev, X. Zhang, M. Walls, M. M.
Murnane, and H. C. Kapteyn, “High flux coherent super-continuum soft X-ray source driven
by a single-stage, 10mJ, Ti:sapphire amplifier-pumped OPA.” Opt. Express 22, 6194–202(2014).
[86] A. L’Huillier, K. J. Schafer, and K. C. Kulander, “Theoretical aspects of intense field harmonic
generation,” J. Phys. B At. Mol. Opt. Phys. 24, 3315–3341 (1999).
[87] G. Sansone, E. Benedetti, F. Calegari, C. Vozzi, L. Avaldi, R. Flammini, L. Poletto, P. Villoresi, C. Altucci, R. Velotta, S. Stagira, S. De Silvestri, and M. Nisoli, “Isolated Single-Cycle
Attosecond Pulses,” Science 314, 443–446 (2006).
[88] I. Christov, M. Murnane, and H. Kapteyn, “High-Harmonic Generation of Attosecond Pulses
in the Single-Cycle Regime,” Phys. Rev. Lett. 78, 1251–1254 (1997).
[89] M.-C. Chen, C. Mancuso, C. Hernández-Garcı́a, F. Dollar, B. Galloway, D. Popmintchev,
P.-C. Huang, B. Walker, L. Plaja, A. A. Jaroń-Becker, A. Becker, M. M. Murnane, H. C.
Kapteyn, and T. Popmintchev, “Generation of bright isolated attosecond soft X-ray pulses
driven by multicycle midinfrared lasers.” Proc. Natl. Acad. Sci. U. S. A. 111, E2361–7 (2014).
[90] S. Wilkins, T. Gureyev, D. Gao, A. Pogany, and A. Stevenson, “Phase-contrast imaging using
polychromatic hard X-rays,” Nature 384, 335–384 (1996).
[91] A. Snigirev, V. Kohn, I. Snigireva, and B. Lengeler, “A compound refractive lens for focusing
high-energy X-rays,” Nature 384, 49–51 (1996).

110[92] A. Snigirev, V. Kohn, I. Snigireva, A. Souvorov, and B. Lengeler, “Focusing high-energy xrays by compound refractive lenses.” Appl. Opt. 37, 653–662 (1998).
[93] A. Schropp, R. Hoppe, V. Meier, J. Patommel, F. Seiboth, H. J. Lee, B. Nagler, E. C. Galtier,
B. Arnold, U. Zastrau, J. B. Hastings, D. Nilsson, F. Uhlén, U. Vogt, H. M. Hertz, and C. G.
Schroer, “Full spatial characterization of a nanofocused x-ray free-electron laser beam byptychographic imaging.” Sci. Rep. 3, 1633 (2013).
[94] F. Seiboth, A. Schropp, R. Hoppe, V. Meier, J. Patommel, H. J. Lee, B. Nagler, E. C. Galtier,
B. Arnold, U. Zastrau, J. B. Hastings, D. Nilsson, F. Uhlén, U. Vogt, H. M. Hertz, and C. G.
Schroer, “Focusing XFEL SASE pulses by rotationally parabolic refractive x-ray lenses,” J.
Phys. Conf. Ser. 499, 1–10 (2014).
[95] A. A. Snigirev, “Refractive lenses allow compact, precision focusing of x-rays,” SPIE Newsroom (2011).
[96] P. Horowitz and J. A. Howell, “A scanning x-ray microscope using synchrotron radiation.”
Science 178, 608–611 (1972).
[97] I. McNulty, J. Kirz, C. Jacobsen, E. H. Anderson, M. R. Howells, and D. P. Kern, “HighResolution Imaging by Fourier Transform X-ray Holography.” Science 256, 1009–1012 (1992).
[98] S. Eisebitt, J. Luning, W. Schlotter, M. Lorgen, O. Hellwig, W. Eberhardt, and J. Stohr,“Lensless imaging of magnetic nanostructures by X-ray spectro-holography,” Nature 432,
885–888 (2004).
[99] P. Kirkpatrick and A. V. Baez, “Formation of optical images by X-rays.” J. Opt. Soc. Am.
38, 766–774 (1948).
[100] I. A. Artioukov, X.-r. O. Group, K. M. Krymski, and M. Region, “Schwarzschild objective
for soft x-rays,” Opt. Eng. 39, 1–8 (2000).
[101] I. A. Artyukov, “Schwarzschild objective and similar two-mirror systems,” Short-Wavelength
Imaging Spectrosc. Sources, Proc. SPIE 8678, 86780A (2012).
[102] A. Budano, F. Flora, and L. Mezi, “Analytical design method for a modified Schwarzschild
optics.” Appl. Opt. 45, 4254–4262 (2006).
[103] S. Bollanti, P. Di Lazzaro, F. Flora, L. Mezi, D. Murra, and a. Torre, “Conventional andmodified Schwarzschild objective for EUV lithography: Design relations,” Appl. Phys. B
Lasers Opt. 85, 603–610 (2006).
[104] S. Matsuyama, H. Nakamori, T. Goto, and T. Kimura, “Nearly diffraction-limited X-ray
focusing with variable-numerical- aperture focusing optical system based on four deformablemirrors,” Sci. Rep. 6, 24801 (2016).
[105] H. Mimura, S. Handa, T. Kimura, H. Yumoto, D. Yamakawa, H. Yokoyama, S. Matsuyama,
K. Inagaki, K. Yamamura, Y. Sano, K. Tamasaku, Y. Nishino, M. Yabashi, T. Ishikawa, andK. Yamauchi, “Breaking the 10nm barrier in hard-X-ray focusing,” Nat. Phys. 6, 122–125(2010).

111[106] H. C. Kang, H. Yan, R. P. Winarski, M. V. Holt, J. Maser, C. Liu, R. Conley, S. Vogt,
A. T. MacRander, and G. B. Stephenson, “Focusing of hard x-rays to 16 nanometers with amultilayer Laue lens,” Appl. Phys. Lett. 92 (2008).
[107] A. J. Morgan, M. Prasciolu, A. Andrejczuk, J. Krzywinski, A. Meents, D. Pennicard,
H. Graafsma, A. Barty, R. J. Bean, M. Barthelmess, D. Oberthuer, O. Yefanov, A. Aquila,
H. N. Chapman, and S. Bajt, “High numerical aperture multilayer Laue lenses.” Sci. Rep. 5,9892 (2015).
[108] M. Prasciolu, a. F. G. Leontowich, J. Krzywinski, a. Andrejczuk, H. N. Chapman, and S. Bajt,“Fabrication of wedged multilayer Laue lenses,” Opt. Mater. Express 5, 748 (2015).
[109] C. Jacobsen, S. Williams, E. Anderson, M. Browne, C. Buckley, D. Kern, J. Kirz, M. Rivers,
and X. Zhang, “Diffraction-limited imaging in a scanning transmission x-ray microscope,”
Opt. Commun. 86, 351–364 (1991).
[110] A. L. D. Kilcoyne, T. Tyliszczak, W. F. Steele, S. Fakra, P. Hitchcock, K. Franck, E. Anderson,
B. Harteneck, E. G. Rightor, G. E. Mitchell, A. P. Hitchcock, L. Yang, T. Warwick, and
H. Ade, “Interferometer-controlled scanning transmission X-ray microscopes at the Advanced
Light Source,” Synchrotron Radiat. News 10, 125–136 (2003).
[111] W. Chao, B. Harteneck, J. Liddle, E. Anderson, and D. Attwood, “Soft X-ray microscopy ata spatial resolution better than 15 nm,” Nature 435, 1210–1213 (2005).
[112] W. Chao, J. Kim, S. Rekawa, P. Fischer, and E. H. Anderson, “Demonstration of 12 nm
resolution Fresnel zone plate lens based soft x-ray microscopy.” Opt. Express 17, 17669–
17677 (2009).
[113] W. Chao, P. Fischer, T. Tyliszczak, S. Rekawa, E. Anderson, and P. Naulleau, “Real space
soft x-ray imaging at 10 nm spatial resolution,” Opt. Express 20, 9777 (2012).
[114] F. Döring, a. L. Robisch, C. Eberl, M. Osterhoff, a. Ruhlandt, T. Liese, F. Schlenkrich,
S. Hoffmann, M. Bartels, T. Salditt, and H. U. Krebs, “Sub-5 nm hard x-ray point focusing
by a combined Kirkpatrick-Baez mirror and multilayer zone plate,” Opt. Express 21, 19311–
19323 (2013).
[115] M. D. De Jonge, B. Hornberger, C. Holzner, D. Legnini, D. Paterson, I. McNulty, C. Jacobsen,
and S. Vogt, “Quantitative phase imaging with a scanning transmission X-ray microscope,”
Phys. Rev. Lett. 100, 1–4 (2008).
[116] A. Sakdinawat and D. Attwood, “Nanoscale X-ray imaging,” Nat. Photonics 4, 840–848(2010).
[117] X. Huang, H. Miao, J. Steinbrener, J. Nelson, D. Shapiro, A. Stewart, J. Turner, and C. Jacobsen, “Signal-to-noise and radiation exposure considerations in conventional and diffraction
x-ray microscopy.” Opt. Express 17, 13541–13553 (2009).
[118] R. W. Gerchberg and W. O. Saxton, “A Practical Algorithm for the Determination of Phasefrom Image and Diffraction Plane Pictures,” Optik (Stuttg). 35, 237–246 (1972).
[119] J. Fienup, “Reconstruction of an object from the modulus of its Fourier transform,” Opt.
Lett. 3, 27–29 (1978).

112[120] J. R. Fienup, “Phase retrieval algorithms: a comparison.” Appl. Opt. 21, 2758–69 (1982).
[121] J. R. Fienup, “Phase retrieval algorithms: a personal tour [Invited].” Appl. Opt. 52, 45–56(2013).
[122] J. Cederquist, J. Fienup, C. Marron, and R. Paxman, “Phase retrieval from experimental
far-field speckle data,” Otpics Lett. 13, 619 (1988).
[123] M. J. Pérez-Ilzarbe, M. Nieto-Vesperinas, and R. Navarro, “Phase retrieval from experimental
far-field intensity data,” J. Opt. Soc. Am. A 7, 434 (1990).
[124] I. K. Robinson, J. L. Libbert, I. a. Vartanyants, J. a. Pitney, D. M. Smilgies, D. L. Abernathy,
and G. Grübel, “Coherent x-ray diffraction imaging of silicon oxide growth,” Phys. Rev. B
60, 9965–9972 (1999).
[125] J. Miao, P. Charalambous, J. Kirz, and D. Sayre, “Extending the methodology of X-ray
crystallography to allow imaging of micrometre-sized non-crystalline specimens,” Nature 400,
342–344 (1999).
[126] H. Mimura, S. Matsuyama, H. Yumoto, H. Hara, K. Yamamura, Y. Sano, M. Shibahara,
K. Endo, Y. Mori, Y. Nishlno, K. Tamasaku, M. Yabashi, T. Ishikawa, and K. Yamauchi,“Hard X-ray diffraction-limited nanofocusing with kirkpatrick-baez mirrors,” Jpn. J. Appl.
Phys. 44, L539 – L542 (2005).
[127] I.-B. Sohn, M. S. Ahsan, Y.-C. Noh, H.-K. Choi, J.-T. Kim, and M.-J. Ko, “Fabrication of
Fresnel zone plate lens in fused silica glass using femtosecond laser lithography technology,”
Opt. Eng. 53, 055107 (2014).
[128] H. N. Chapman and K. A. Nugent, “Coherent lensless X-ray imaging,” Nat. Photonics 4,
833–839 (2010).
[129] J. Miao, R. L. Sandberg, and C. Song, “Coherent X-ray diffraction imaging,” IEEE J. Sel.
Top. Quant. Electron 18, 399–410 (2011).
[130] D. Sayre, “Some implications of a theorem due to Shannon,” Acta Crystallogr. 5, 843–843(1952).
[131] C. E. Shannon, “Communication in the Presence of Noise,” Proc. IEEE 86, 447–457 (1998).
[132] V. Elser, “Phase retrieval by iterated projections,” J. Opt. Soc. Am. A 20, 40–55 (2003).
[133] S. Marchesini, H. He, H. N. Chapman, S. P. Hau-Riege, A. Noy, M. R. Howells, U. Weierstall,and J. C. H. Spence, “X-ray image reconstruction from a diffraction pattern alone,” Phys.
Rev. B 68, 140101 (2003).
[134] D. R. Luke, “Relaxed Averaged Alternating Reflections for Diffraction Imaging,” Inverse
Probl. 37, 13 (2004).
[135] S. T. Thurman and J. R. Fienup, “Phase retrieval with signal bias.” J. Opt. Soc. Am. A.
Opt. Image Sci. Vis. 26, 1008–14 (2009).

113[136] D. E. Adams, L. S. Martin, M. D. Seaberg, D. F. Gardner, H. C. Kapteyn, and M. M.
Murnane, “A generalization for optimized phase retrieval algorithms,” Opt. Express 20, 24778(2012).
[137] M. Seaberg, D. Adams, E. Townsend, D. Raymondson, W. Schlotter, Y. Liu, C. Menoni,
L. Rong, C. Chen, J. Miao, H. Kapteyn, and M. Murnane, “Ultrahigh 22 nm resolution
coherent diffractive imaging using a desktop 13 nm high harmonic source,” Opt. Express 19,
22470–9 (2011).
[138] J. W. Goodman, Introduction to Fourier Optics (Roberts and Company Publishers, Greenwood Village, 2005), 3rd ed.
[139] J. Miao and D. Sayre, “On possible extensions of X-ray crystallography through diffractionpattern oversampling research papers On possible extensions of X-ray crystallography throughdiffraction-pattern oversampling,” Acta Crystallogr. A56, 596–605 (2000).
[140] J. Miao, D. Sayre, and H. N. Chapman, “Phase retrieval from the magnitude of the Fouriertransforms of nonperiodic objects,” J. Opt. Soc. Am. A 15, 1662 (1998).
[141] J. Miao, T. Ishikawa, E. Anderson, and K. Hodgson, “Phase retrieval of diffraction patterns
from noncrystalline samples using the oversampling method,” Phys. Rev. B 67, 174104 (2003).
[142] C. Song, D. Ramunno-Johnson, Y. Nishino, Y. Kohmura, T. Ishikawa, C.-C. Chen, T.-K.
Lee, and J. Miao, “Phase retrieval from exactly oversampled diffraction intensity throughdeconvolution,” Phys. Rev. B 75, 012102 (2007).
[143] W. Hoppe, “Beugung im inhomogenen Primärstrahlwellenfeld,” Acta Crystallogr. Sect. A
25, 495–515 (1969).
[144] J. M. Rodenburg, “Ptychography and related diffractive imaging methods,” Adv. Imaging
Electron Phys. 150, 87–184 (2008).
[145] J. Rodenburg, “Ptychography: early history and 3D scattering effects,” in “Proc. SPIE ShortWavelength Imaging Spectrosc. Sources,” , vol. 8678 (2012), vol. 8678, pp. 1–10.
[146] B. C. McCallum and J. M. Rodenburg, “Two-dimensional demonstration of Wigner phaseretrieval microscopy in the STEM configuration,” Ultramicroscopy 45, 371–380 (1992).
[147] H. Faulkner and J. Rodenburg, “Movable Aperture Lensless Transmission Microscopy: A
Novel Phase Retrieval Algorithm,” Phys. Rev. Lett. 93, 023903 (2004).
[148] J. M. Rodenburg and H. M. L. Faulkner, “A phase retrieval algorithm for shifting illumination,” Appl. Phys. Lett. 85, 4795 (2004).
[149] P. Thibault, M. Dierolf, A. Menzel, O. Bunk, C. David, and F. Pfeiffer, “High-resolution
scanning x-ray diffraction microscopy.” Science 321, 379–82 (2008).
[150] A. Maiden and J. Rodenburg, “An improved ptychographical phase retrieval algorithm for
diffractive imaging,” Ultramicroscopy 109, 1256–62 (2009).
[151] J. Rodenburg and R. H. T. Bates, “The theory of super-resolution electron microscopy via
Wigner-distribution deconvolution,” Phil. Trans. R. Soc. Lond. A 336, 521–553 (1992).

114[152] M. Humphry, B. Kraus, a.C. Hurst, a.M. Maiden, and J. Rodenburg, “Ptychographic electron
microscopy using high-angle dark-field scattering for sub-nanometre resolution imaging,” Nat.
Commun. 3, 730 (2012).
[153] J. C. H. Spence, U. Weierstall, and M. Howells, “Coherence and sampling requirements for
diffractive imaging.” Ultramicroscopy 101, 149–52 (2004).
[154] P. Thibault, M. Dierolf, O. Bunk, A. Menzel, and F. Pfeiffer, “Probe retrieval in ptychographic
coherent diffractive imaging,” Ultramicroscopy 109, 338–43 (2009).
[155] X. Huang, H. Yan, R. Harder, Y. Hwu, I. K. Robinson, and Y. S. Chu, “Optimization of
overlap uniformness for ptychography,” Opt. Express 22, 12634 (2014).
[156] M. Guizar-Sicairos and J. Fienup, “Phase retrieval with transverse translation diversity: anonlinear optimization approach,” Opt. Express 16, 7264–7278 (2008).
[157] P. Thibault and M. Guizar-Sicairos, “Maximum-likelihood refinement for coherent diffractive
imaging,” New J. Phys. 14, 1–20 (2012).
[158] C. T. Putkunz, J. N. Clark, D. J. Vine, G. J. Williams, M. A. Pfeifer, E. Balaur, I. McNulty,
K. A. Nugent, and A. G. Peele, “Phase-diverse coherent diffractive imaging: High sensitivity
with low dose,” Phys. Rev. Lett. 106, 1–4 (2011).
[159] J. R. Fienup, “Invariant error metrics for image reconstruction.” Appl. Opt. 36, 8352–8357(1997).
[160] S. Marathe, S. S. Kim, S. N. Kim, C. Kim, H. C. Kang, P. V. Nickles, and D. Y. Noh,
“Coherent diffraction surface imaging in reflection geometry,” Opt. Express 18, 7253–62(2010).
[161] S. Roy, D. Parks, K. A. Seu, R. Su, J. J. Turner, W. Chao, E. H. Anderson, S. Cabrini, andS. D. Kevan, “Lensless X-ray imaging in reflection geometry,” Nat. Photonics 5, 243–245(2011).
[162] T. Sun, Z. Jiang, J. Strzalka, L. Ocola, and J. Wang, “Three-dimensional coherent X-ray
surface scattering imaging near total external reflection,” Nat. Photonics 6, 586 –590 (2012).
[163] T. Harada, M. Nakasuji, Y. Nagata, T. Watanabe, and H. Kinoshita, “Phase Imaging ofExtreme-Ultraviolet Mask Using Coherent Extreme-Ultraviolet Scatterometry Microscope,”
Jpn. J. Appl. Phys. 52, 06GB02 (2013).
[164] M. Zürch, C. Kern, and C. Spielmann, “XUV coherent diffraction imaging in reflection geometry with low numerical aperture,” Opt. Express 21, 21131–21147 (2013).
[165] D. F. Gardner, B. Zhang, M. D. Seaberg, L. S. Martin, D. E. Adams, F. Salmassi, E. Gullikson, H. Kapteyn, and M. Murnane, “High numerical aperture reflection mode coherent diffraction microscopy using off-axis apertured illumination,” Opt. Express 20, 19050–9 (2012).
[166] J. W. Cooley and J. W. Tukey, “An Algorithm for Machine Calculation of Complex Fourier
Series,” Math. Comput. 19, 297–301 (1965).
[167] M. Frigo and S. G. Johnson, “The design and implementation of FFTW3,” Proc. IEEE 93,
216–231 (2005).

115[168] B. Zhang, D. F. Gardner, M. D. Seaberg, E. R. Shanblatt, H. C. Kapteyn, M. M. Murnane,
and D. E. Adams, “High contrast 3D imaging of surfaces near the wavelength limit using
tabletop EUV ptychography,” Ultramicroscopy 158, 98–104 (2015).
[169] M. Seaberg, B. Zhang, D. Gardner, E. Shanblatt, M. Murnane, H. Kapteyn, and D. Adams,“Tabletop Nanometer Extreme Ultraviolet Imaging in an Extended Reflection Mode Using
Coherent Fresnel Ptychography : supplementary material,” Optica 1, 1–4 (2014).
[170] F. Zhang, I. Peterson, J. Vila-Comamala, A. Diaz, F. Berenguer, R. Bean, B. Chen, A. Menzel, I. Robinson, and J. Rodenburg, “Translation position determination in ptychographic
coherent diffraction imaging,” Opt. Express 21, 13592–13606 (2013).
[171] D. Shapiro, P. Thibault, T. Beetz, V. Elser, M. Howells, C. Jacobsen, J. Kirz, E. Lima,
H. Miao, A. M. Neiman, and D. Sayre, “Biological imaging by soft x-ray diffraction microscopy.” Proc. Natl. Acad. Sci. U. S. A. 102, 15343–6 (2005).
[172] H. N. Chapman, A. Barty, S. Marchesini, A. Noy, S. P. Hau-riege, C. Cui, M. R. Howells,
R. Rosen, H. He, J. C. H. Spence, U. Weierstall, T. Beetz, C. Jacobsen, and D. Shapiro,“High-resolution ab initio three-dimensional x-ray diffraction microscopy,” J. Opt. Soc. Am.
A 23 (2006).
[173] D. F. Gardner, M. Tanksalvala, E. R. Shanblatt, X. Zhang, B. R. Galloway, C. L. Porter,
R. Karl-Jr., C. Bevis, D. E. Adams, H. C. Kapteyn, M. M. Murnane, and G. F. Mancini, “Subwavelength coherent imaging of periodic samples using a 13.5 nm tabletop high harmonic lightsource,” Submitted (2016).
[174] P. Thibault, M. Dierolf, A. Menzel, O. Bunk, C. David, and F. Pfeiffer, “High-resolution
scanning x-ray diffraction microscopy,” Science 321, 379–82 (2008).
[175] D. Sayre, “Prospects for long wavelength X-Ray microscopy and diffraction,” in “Imaging
Process. coherence Phys.”, , vol. 112 (1980), vol. 112, pp. 229–235.
[176] R. W. Falcone and J. Bokor, “Dichroic beam splitter for extreme-ultraviolet and visible
radiation,” Opt. Lett. 8, 21–23 (1983).
[177] Y. Nagata, Y. Nabekawa, and K. Midorikawa, “Development of high-throughput, highdamage-threshold beam separator for 13 nm high-order harmonics.” Opt. Lett. 31, 1316–1318(2006).
[178] S. Ichimaru, M. Hatayama, T. Ohchi, E. M. Gullikson, and S. Oku, “Performance of aruthenium beam separator used to separate soft x rays from light generated by a high-orderharmonic light source,” Appl. Opt. 55, 984–988 (2016).
[179] E. R. Shanblatt, C. L. Porter, D. F. Gardner, G. F. Mancini, R. M. Karl, M. D. Tanksalvala,
C. S. Bevis, V. H. Vartanian, H. C. Kapteyn, D. E. Adams, and M. M. Murnane, “Quantitative Chemically-Specific Coherent Diffractive Imaging of Buried Interfaces using a Tabletop
EUV Nanoscope,” Nano Lett. 19, 5444–5450 (2016).
[180] B. L. Henke, E. M. Gullikson, and J. C. Davis, “X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92,” At. Data Nucl. Data
Tables 54, 181–342 (1993).

116[181] A. M. Maiden, M. J. Humphry, F. Zhang, and J. M. Rodenburg, “Superresolution imaging
via ptychography.” J. Opt. Soc. Am. A 28, 604–612 (2011).
[182] M. Odstrcil, J. Bussmann, D. Rudolf, R. Bresenitz, J. Miao, W. S. Brocklesby, and
L. Juschkin, “Ptychographic imaging with a compact gasdischarge plasma extreme ultraviolet light source,” Opt. Lett. 40, 5574–5577 (2015).
[183] P. Thibault and A. Menzel, “Reconstructing state mixtures from diffraction measurements.”
Nature 494, 68–71 (2013).
[184] D. J. Batey, D. Claus, and J. M. Rodenburg, “Information multiplexing in ptychography,”
Ultramicroscopy 138, 13–21 (2013).
[185] T. B. Edo, D. J. Batey, a. M. Maiden, C. Rau, U. Wagner, Z. D. Pešić, T. a. Waigh, andJ. M. Rodenburg, “Sampling in x-ray ptychography,” Phys. Rev. A - At. Mol. Opt. Phys.
87, 1–8 (2013).
[186] D. J. Batey, T. B. Edo, C. Rau, U. Wagner, Z. D. Pesic, T. A. Waigh, and J. M. Rodenburg,“Reciprocal-space up-sampling from real-space oversampling in x-ray ptychography,” Phys.
Rev. A - At. Mol. Opt. Phys. 89, 1–5 (2014).
[187] A. M. Maiden, M. J. Humphry, and J. M. Rodenburg, “Ptychographic transmission microscopy in three dimensions using a multi-slice approach.” J. Opt. Soc. Am. A 29, 1606–1614(2012).
[188] T. M. Godden, R. Suman, M. J. Humphry, J. M. Rodenburg, and A. M. Maiden, “Ptychographic microscope for three-dimensional imaging,” Opt. Express 22, 12513–12523 (2014).
[189] A. Suzuki, S. Furutaku, K. Shimomura, K. Yamauchi, Y. Kohmura, T. Ishikawa, and Y. Takahashi, “High-resolution multislice X-ray ptychography of extended thick objects,” Phys. Rev.
Lett. 112, 1–5 (2014).
[190] K. Shimomura, A. Suzuki, M. Hirose, and Y. Takahashi, “Precession x-ray ptychography withmultislice approach,” Phys. Rev. B - Condens. Matter Mater. Phys. 91, 1–5 (2015).
[191] K. M. Hoogeboom-Pot, J. N. Hernandez-Charpak, E. H. Anderson, X. Gu, R. Yang, M. M.
Murnane, H. C. Kapteyn, and D. Nardi, “A new regime of nanoscale thermal transport:collective diffusion counteracts dissipation inefficiency,” PNAS 112, 4846–4851 (2015).
[192] D. D. Hickstein, F. Dollar, J. A. Gaffney, M. E. Foord, G. M. Petrov, B. B. Palm, K. E.
Keister, J. L. Ellis, C. Ding, S. B. Libby, J. L. Jimenez, H. C. Kapteyn, M. M. Murnane, andW. Xiong, “Observation and control of shock waves in individual nanoplasmas,” Phys. Rev.
Lett. 112, 1–5 (2014).
[193] S. Mathias, C. La-O-Vorakiat, J. M. Shaw, E. Turgut, P. Grychtol, R. Adam, D. Rudolf,
H. T. Nembach, T. J. Silva, M. Aeschlimann, C. M. Schneider, H. C. Kapteyn, and M. M.
Murnane, “Ultrafast element-specific magnetization dynamics of complex magnetic materials
on a table-top,” J. Electron Spectros. Relat. Phenomena 189, 164–170 (2013).
[194] E. Turgut, C. La-O-Vorakiat, J. M. Shaw, P. Grychtol, H. T. Nembach, D. Rudolf, R. Adam,
M. Aeschlimann, C. M. Schneider, T. J. Silva, M. M. Murnane, H. C. Kapteyn, and S. Mathias, “Controlling the competition between optically induced ultrafast spin-flip scattering andspin transport in magnetic multilayers,” Phys. Rev. Lett. 110, 197201 (2013).

117[195] M. Murnane and J. Miao, “Optics: Ultrafast X-ray photography,” Nature 460, 1088–90(2009).
[196] H. N. Chapman, S. P. Hau-Riege, M. J. Bogan, S. Bajt, A. Barty, S. Boutet, S. Marchesini,
M. Frank, B. W. Woods, W. H. Benner, R. a. London, U. Rohner, A. Szöke, E. Spiller,
T. Möller, C. Bostedt, D. a. Shapiro, M. Kuhlmann, R. Treusch, E. Plönjes, F. Burmeister,M. Bergh, C. Caleman, G. Huldt, M. M. Seibert, and J. Hajdu, “Femtosecond time-delay
X-ray holography.” Nature 448, 676–9 (2007).
[197] A. A. Khorshad, K. Hassani, and M. T. Tavassoly, “Nanometer displacement measurement
using Fresnel diffraction.” Appl. Opt. 51, 5066–72 (2012).
[198] S. Carbajo, I. D. Howlett, F. Brizuela, K. S. Buchanan, M. C. Marconi, W. Chao, E. H.
Anderson, I. Artioukov, a. Vinogradov, J. J. Rocca, and C. S. Menoni, “Sequential singleshot imaging of nanoscale dynamic interactions with a table-top soft x-ray laser.” Opt. Lett.
37, 2994–6 (2012).
[199] A. Barty, S. Boutet, M. J. Bogan, S. Hau-Riege, S. Marchesini, K. Sokolowski-Tinten, N. Stojanovic, R. Tobey, H. Ehrke, A. Cavalleri, S. Düsterer, M. Frank, S. Bajt, B. W. Woods, M. M.
Seibert, J. Hajdu, R. Treusch, and H. N. Chapman, “Ultrafast single-shot diffraction imagingof nanoscale dynamics,” Nat. Photonics 2, 415–419 (2008).
[200] a. Ravasio, D. Gauthier, F. R. N. C. Maia, M. Billon, J. P. Caumes, D. Garzella, M. Géléoc,
O. Gobert, J. F. Hergott, a. M. Pena, H. Perez, B. Carré, E. Bourhis, J. Gierak, A. Madouri,
D. Mailly, B. Schiedt, M. Fajardo, J. Gautier, P. Zeitoun, P. H. Bucksbaum, J. Hajdu, and
H. Merdji, “Single-shot diffractive imaging with a table-top femtosecond soft X-ray laserharmonics source,” Phys. Rev. Lett. 103, 028104 (2009).
[201] K. W. DeLong, R. Trebino, J. Hunter, and W. E. White, “Frequency-resolved optical gatingwith the use of second-harmonic generation,” J. Opt. Soc. Am. B 11, 2206 (1994).
[202] Q. Li, K. Hoogeboom-Pot, D. Nardi, M. M. Murnane, H. C. Kapteyn, M. E. Siemens, E. H.
Anderson, O. Hellwig, E. Dobisz, B. Gurney, R. Yang, and K. A. Nelson, “Generation andcontrol of ultrashort-wavelength two-dimensional surface acoustic waves at nanoscale interfaces,” Phys. Rev. B - Condens. Matter Mater. Phys. 85, 195431 (2012).
[203] K. M. Hoogeboom-Pot, E. Turgut, J. N. Hernandez-Charpak, J. M. Shaw, H. C. Kapteyn,
M. M. Murnane, and D. Nardi, “Nondestructive Measurement of the Evolution of LayerSpecific Mechanical Properties in Sub-10 nm Bilayer Films,” Nano Lett. 16, 4773–4778 (2016).
[204] J. H. Underwood and T. W. Barbee, “Layered synthetic microstructures as Bragg diffractors
for X rays and extreme ultraviolet: theory and predicted performance,” Appl. Opt. 20, 3027
(1981).
[205] O. Kfir, P. Grychtol, E. Turgut, R. Knut, D. Zusin, D. Popmintchev, T. Popmintchev,
H. Nembach, J. M. Shaw, A. Fleischer, H. Kapteyn, M. Murnane, and O. Cohen, “Generation of bright phase-matched circularly-polarized extreme ultraviolet high harmonics,”
Nat. Photonics pp. 1–7 (2014).
[206] D. D. Hickstein, F. J. Dollar, P. Grychtol, J. L. Ellis, R. Knut, C. Hernández-Garcı́a, D. Zusin,
C. Gentry, J. M. Shaw, T. Fan, K. M. Dorney, A. Becker, A. Jaroń-Becker, H. C. Kapteyn,118
M. M. Murnane, and C. G. Durfee, “Non-collinear generation of angularly isolated circularly
polarized high harmonics,” Nat. Photonics 9 (2015).
[207] A. Tripathi, J. Mohanty, S. H. Dietze, O. G. Shpyrko, E. Shipton, E. E. Fullerton, S. S. Kim,and I. McNulty, “Dichroic coherent diffractive imaging.” Proc. Natl. Acad. Sci. U. S. A. 108,
13393–8 (2011).
[208] C. Donnelly, V. Scagnoli, M. Guizar-Sicairos, M. Holler, F. Wilhelm, F. Guillou, A. Rogalev,
C. Detlefs, A. Menzel, J. Raabe, and L. J. Heyderman, “High Resolution Hard X-ray Magnetic
Imaging with Dichroic Ptychography,” Phys. Rev. B 064421, 1–5 (2016).
[209] S. Zayko, E. Mönnich, M. Sivis, D.-D. Mai, T. Salditt, S. Schäfer, and C. Ropers, “Coherent
diffractive imaging beyond the projection approximation: waveguiding at extreme ultraviolet
wavelengths,” Opt. Express 23, 19911 (2015).
[210] S. O. Kim, H. H. Solak, M. P. Stoykovich, N. J. Ferrier, J. J. De Pablo, and P. F. Nealey,“Epitaxial self-assembly of block copolymers on lithographically defined nanopatterned substrates.” Nature 424, 411–4 (2003).
[211] B. Zhang, D. F. Gardner, M. D. Seaberg, E. R. Shanblatt, C. Porter, R. Karl-Jr., C. Mancuso, H. C. Kapteyn, M. M. Murnane, and D. E. Adams, “Ptychographic Hyperspectral
Spectromicroscopy with an Extreme Ultraviolet High Harmonic Comb,” Opt. Express 24,
18745 (2016).
[212] R. Karl, C. Bevis, R. Lopez-Rios, J. Reichanadter, D. Gardner, C. Porter, E. Shanblatt,
M. Tanksalvala, G. F. Mancini, M. Murnane, H. Kapteyn, and D. Adams, “Spatial, spectral,and polarization multiplexed ptychography,” Opt. Express 23, 30250–30258 (2015).
[213] A. Fleischer, O. Kfir, T. Diskin, P. Sidorenko, and O. Cohen, “Spin angular momentum andtunable polarization in high-harmonic generation,” Nat. Photonics 8, 543–549 (2014).
[214] X. Shi, P. Fischer, V. Neu, D. Elefant, J. C. T. Lee, D. A. Shapiro, M. Farmand, T. Tyliszczak,
H. W. Shiu, S. Marchesini, S. Roy, and S. D. Kevan, “Soft x-ray ptychography studies ofnanoscale magnetic and structural correlations in thin SmCo5 films,” Appl. Phys. Lett. 108(2016).
[215] B. Zhang, D. F. Gardner, M. D. Seaberg, E. R. Shanblatt, C. Porter, R. Karl-Jr., C. Mancuso,
H. C. Kapteyn, M. M. Murnane, and D. E. Adams, “Ptychographic Hyperspectral Spectromicroscopy with an Extreme Ultraviolet High Harmonic Comb,” Opt. Express 24, 98–104(2016).
[216] U. O. Edinburgh, “Topic 2: Scalar Diffraction,” http://www2.ph.ed.ac.uk/˜wjh/teaching/mo/slides/scalar/scalar.pdf Autumn Ter.
[217] J. M. Cowley, Diffraction Physics (Elsevier Science B.V., New York, 1995), 3rd ed.

Appendix A

From Maxwell to Fraunhofer

In coherent diffractive imaging (CDI), it is assumed the diffracted light collected on thedetector is proportional to the Fourier Transform of the object. In this appendix, the assumptions
and their applicability are discussed. Starting with Maxwell’s equations in vacuum, the wave
equation is derived. Then using a Green’s function approach, the outline of a derivation is given
to model the diffraction from an aperture. In the end, an expression for Fresnel and Fraunhofer
diffraction is given with comments on their appropriate use. 1

A.1

The Wave Equation from Maxwell’s Equations
Due to EUV absorption by atmosphere, the EUV imaging demonstrations are in vacuum(10−6 Torr) in the absence of free charge, thus simplifying Maxwell’s equations to~~ = −µ0 ∂ H
∇×E
∂t

(A.1)

~
∂E
∂t

(A.2)

~ =0
∇ · 0 E

(A.3)

~ =0
∇ · µ0 H(A.4)~ = 0∇×H

1

The notation and derivation presented here closely follows Goodman [138]120~ is the electric field, H~ is the magnetic field, µ0 is the permeability of free space, and 0
where Eis the permittivity of free space. Applying the curl operator (∇×) to Eq. A.1 and switching theorder of the time and space derivatives yields~~ = −µ0 ∂(∇ × H) .
∇×∇×E
∂t

(A.5)

~ = ∇(∇ · E)
~ − ∇2 E)~ and substituting in Eq.
The application of the vector identity ∇ × (∇ × E)
A.2 gives the following wave equation
~−
∇2 E

~
1 ∂2E
=0
2
2
c ∂t

(A.6)

where c is the speed of light given by1c= √.
µ 0 0(A.7)

The same procedure can be done with the magnetic field resulting in
~ −
∇2 H

~
1 ∂2H
= 0.
2
c ∂t2

(A.8)

In a vacuum, the medium is linear, isotropic, homogeneous, and non-dispersive, therefore
each x, y and z component of the electric and magnetic fields can be described by single scalar
wave equation:
1 ∂2u
= 0.
c2 ∂t2(A.9)

u = Re[U (P )e−i2πνt ](A.10)∇2 u −The solution iswhere Re[ ] signifies the real part and U (P ) is a complex function of position given by
U (P ) = A(P )eiφ(P )(A.11)

where ν is the frequency, A(P ) is the amplitude, and φ(P ) is the phase. Both A(P ) and φ(P ) are
functions of position, P . Writing the solution using U(P) allows spatial and temporal dependence
to be separated. Plugging in Eq. A.10 into Eq. A.9 yields the Helmholtz equation:(∇2 + k 2 )U = 0(A.12)

121
withk = 2πν
2π=cλ(A.13)

where λ is the wavelength. The monochromatic plane wave, U = U0 ei(kx−ωt) , is a solution, with
ω = 2πν, but a more complex solution is needed to describe the diffraction from an arbitrary
waveform through an arbitrary planar screen.

A.2

Diffraction by a Planar Screen
To calculate the diffraction by a planar screen, Green’s theorem is used and is stated asfollows:
Z Z Z


Z Z 
∂G ∂U
−
ds
(U ∇ G − G∇ U )dv =
U
∂n
∂n
V
S
2

2

(A.14)

where V is a volume, S is a closed surface, ∂/∂n points in the outward normal direction, and G
is an auxiliary function, or Green s function, which needs to be carefully chosen. The first Greenfunction considered is the free space Green’s function,
GK =eikr01,
r01(A.15)

which used by Kirchhoff to solve for the diffraction from a point source through an aperture ina planar screen, where r01 is the magnitude of the vector ~r01 that points from P0 to P1 (see Fig.
A.1).
Using the free space Green’s function leads internal inconsistencies in the boundary conditions. To avoid inconsistencies, Rayleigh-Sommerfeld used the following Green’s functions:G− =eikr01eikr̃01−
r01
r̃01(A.16)

G+ =eikr01eikr̃01+
r01
r̃01(A.17)In these Green’s functions a mirror point is used on the opposite side of the screen from P0 (seeFig. A.2) with r̃01 is the length of the vector from P̃0 to P1 .

122

Figure A.1: Diffraction from Planar Screen from a Point Source

Figure A.2: Mirror Point Source123
Using Green’s Theorem (Eq. A.14) and the above choices of Green’s functions leads toA
U (P0 ) =iλZ Zeik(r21 +r01 )Ψds
r21 r01
Σ(A.18)

where A is the amplitude of the point source, and Σ is the open area in the screen, and Ψ is theobliquity factor and depends of the choice of green function. Using the free space Green’s function,
as used in the Kirchhoff approach, results inΨ=1
cos(~n, ~r01 ) − cos(~n, ~r21 )2(A.19)

while using the Rayleigh-Sommerfeld Green’s function results inΨ = cos(~n, ~r01 )(A.20)

Ψ = − cos(~n, ~r21 )(A.21)

andfor the G− and G+ , respectively. As long as the wave is observed many wavelengths away fromthe aperture, and the aperture is is much greater than the wavelength, there is negligible difference
between the obliquity factors. Instead of point sources, attention is turned towards an arbitrary
wavefront incident on the aperture.

A.3

Huygens Principle
With inspiration from Huygens principle - each point of a wavefront can be described by aspherically expanding wave - the wavefront incident on the screen at the opening can be describedby a superposition of spherically expanding waves. As discussed above, the obliquity factors arenearly identical if we are far enough away from the aperture, thus we chose the obliquity factor
from the use of the G− Green’s function. Huygens principle is given by
U (P0 ) =

1
iλ

Z Z
U (P1 )
Σ

eikr01cos θds
r01(A.22)

where U (P1 ) is given by Eq. A.11. For numerical calculations, it’s easier to work in Cartesian
coordinates. Following Fig. A.3, the diffracting screen is placed in the (ξ, η) plane and perpendicular

124

Figure A.3: Diffraction Geometry in Cartesian Coordinates

to the z axis. The detection plane lies in the (x, y) plane and we assume the light is incident fromthe left. With this geometry the cosine term is given bycos θ =zr01

(A.23)and Huygens Eq. A.22 can be written as
eikr012 dξdη
r01(A.24)

z 2 + (x − ξ)2 + (y − η)2 .

(A.25)z
U (P0 ) =iλZ ZU (ξ, η)Σwhere the distance between P1 and P0 is
r01 =

A.4

p

The Fresnel Approximation
In the Fresnel approximation, r01 is approximated with a binomial expansion resulting in1  x − ξ 2 1  y − η  2
r01 ≈ z 1 +
+
.
2
z
2
z

(A.26)

Plugging in the approximation of r01 into Eq. A.24 and assuming no light is transmitted outsideof the aperture Σ yields the Fresnel diffraction integral:eikz i k (x2 +y2 )U (x, y) =
e 2z
iλz

Z Z +∞ no 2πk22
U (ξ, η)ei 2z (ξ +η ) e−i λz (xξ+yη) dξdη.
−∞(A.27)

125
This equation can be written in a more illuminating fashion as followshi
U (x, y) = A(x, y)F̂ B(ξ, η)U (ξ, η)(A.28)

where F̂ is the Fourier transform with A and B multiplicative factors. This form of the Fresnel
integral is particularly useful for computational techniques because the Fourier transform can beaccomplished with the efficient, and discrete, Fast Fourier Transform routine [166, 167].
The accuracy of the Fresnel approximation depends on the contribution from higher orderterms in the binomial expansion of Eq. A.25. A strict condition for accuracy is satisfied as long as
z3 

A.5

2
π
(x − ξ)2 + (y − η)2 max
4λ(A.29)

Fraunhofer Diffraction
The Fraunhofer approximation is valid when observing the diffraction in the far-field suchthat the curvature of the wavefront incident on the screen is negligible. This is valid ifzk(ξ 2 + η 2 )max.
2

(A.30)

When the approximation is valid, the multiplicative factor B in the Fresnel integral (Eq. A.28)
goes to one, giving the Fraunhofer diffraction formula:hi
U (x, y) = A(x, y)F̂ U (ξ, η) .

(A.31)

Fraunhofer diffraction is the Fourier Transform of the of the field at the aperture, evaluated at
frequencies fx = x/λz and fy = y/λz , again allowing the use of the Fast Fourier Transform routine(CITE).

A.6

Angular Spectrum of Plane Waves
The angular spectrum of plane wave propagation method is used to discribe the diffraction

between two planes, as shown in Fig. A.4. In this method, the Helmholtz equation is applied to
the Fourier transform of the waveform and a propagator is defined. 2
2

The derivation and notation here closely follows Ref. [216]126

Figure A.4: Angular Spectrum Propagation Between Two Planes

127
To begin, it is assumed the wavefront at the z = 0 plane (u0 (ξ, η)) is known. The Fourier
Transform at the unknown plane is taken, given by
Z Z
U1 (u, v, z) =u1 (x, y, z)e−i2π(ux+vy) dxdy

(A.32)U1 (u, v, z)ei2π(ux+vy) dudv

(A.33)

with the inverse transform given by
Z Z
u1 (x, y, z) =From Eq. A.33, and Fourier transform theory, it is seen that u1 (x, y, z) is composed of a linear
combination of U1 (u, v, z)ei2π(ux+vy) , which must also be a solution to the Helmholtz equation, Eq.
A.12, and results in the following expression (again with k = 2π/λ):∇2 + k U1 (u, v, z)ei2π(ux+vy) = 0(A.34)

Application of the Laplace operator results in∂ 2 U1+ (2πγ)2 U1 = 0∂z z(A.35)

with
r
γ=

1
− u2 − v 2 .
λ2(A.36)

This differential equation can be solved with the initial condition of U0 given by
Z Z
U0 (u, v, 0) =u0 (ξ, η, 0)e−i2π(ξu+ηv) dξdη = F [u0 ].

(A.37)

Using the initial condition, the solution to Eq. A.35 isU1 (u, v, z) = F [u0 ]ei2πγz .

(A.38)

Now taking the inverse Fourier transform
Z Z
u1 (x, y, z) =F [u0 ]ei2πγz ei2π(ux+vy) dudv,(A.39)

which can be written ashiu1 (x, y, z) = F −1 F [u0 ]ei2πγz .

(A.40)

128
From this expression, the field at the second plane, P1 , can be calculated from the first plane P0
using Fourier Transforms and a propagation function in frequency space:H(u, v, z) = ei2πγz .

(A.41)At large z distances, the propagation function becomes highly oscillatory an cannot be sampled properly for numerical calculations. The angular spectrum of plane wave method is best fornear field calculations.

A.7

Propagation Applicability and the Fresnel Number
In this appendix, three methods of wavefront propagation have been discussed. The applica-

bility of each, in practice, can be characterized by the Fresnel number, given by
F =

a2
Lλ

(A.42)

where a is the characteristic size of the aperture, L is the distance from the diffracting screen to theobservation plane, and λ is the wavelength. When F  1, the near-field, use the angular spectrumof plane wave method. When F ∼ 1 use Fresnel propagation. And when F  1, use the far-fieldapproximation of Fraunhofer.

Appendix B

Tilted Plane Correction

When collecting diffraction patterns from a sample at high numerical aperture, there is a
non-linear mapping of frequencies onto the detector. If the sample normal is not parallel to theincident beam, then the mapping is also asymmetrical. The tilted plane correction algorithm remaps the collected diffraction patterns such that the frequencies are sampled on a linear grid.
The re-mapping allows the use of the Fast Fourier Transform algorithms [166, 167] to propagate
between the object and detector plane greatly increasing the reconstruction speed of the phaseretrieval algorithms [165, 168, 169, 179].

B.1

Normal Incidence Geometry
Before considering the non-normal geometry, normal incidence illumination is described first.

Figure B.1a shows the coordinate system used. The sample, S, lies in the (x0 , y 0 ) plane with theincident illumination pointing in the ẑ 0 direction. The normal vector of the sample, n̂s also points
in the ẑ 0 direction. Points within the sample plane are described with polar coordinates: ~r0 and φ.
The detector, D, is parallel to the sample plane, and lies in the (x, y) plane. The normal
vector of the detector, n̂D points in the negative ẑ direction. The distance from the center of thesample to the center of the detector is given by R. The origin of the detector coordinate system isat the center of the sample.

130

Figure B.1: Coordinate Definitions a) The coordinate system used for a normally incident
illumination. b) The coordinate system used for a non-normal incident illumination. Figure adaptedfrom Gardner et al. [165]

131

B.2

Scattering with Normal Incidence Illumination
The far-field diffracted pattern, f (~q), can be described by the first Born appropriation,f (~q) =

µ
4π

Z

0

Φ(~r0 )e−2πi~q·~r d~r0

(B.1)

where µ describes the strength of the interaction with the potential Φ, and ~q is the momentum
transfer vector [217]. The momentum transfer vector is the incident wave vector subtracted fromthe scattered vector: ~q = ~kf − ~ki . The angle between ~kf and ~ki is θ.
Due to conversation of momentum, and the assumed elastic scattering, the magnitude of ~kf
and ~ki are the same, |~k| = 2π/λ = k0 , where λ is the wavelength of illumination. Therefore, thescattered light lies on a spherical surface, which is called the Ewald sphere (see Fig. B.1). The
mapping of the Ewald sphere onto a flat detector is the origin of the non-linear mapping, whichbecomes more evident with increasing numerical aperture.
The momentum transfer vector, when ~ki = k0 ẑ, is written in the detector coordinate systemas~q(x, y, z) = k0 cos φ sin θx̂ + sin φ sin θŷ + (cos θ − 1)ẑ .

(B.2)

If the diffraction is collected at low NA, the small angle approximation can be used for theta, giving~q = k0 cos φx̂ + sin φŷ .

(B.3)

and results in a linear mapping of ~q onto the detector plane as shown in Fig. B.2. On the other
hand, if high NA data is collected, then the mapping is linear in sinθ (Eq. B.2) as shown in Fig.
B.3.
In order to remap the diffraction pattern into linear frequency, ~q is written in detector Cartesian coordinates.
~q = k0 pxx2 + y 2 + R 2

x̂ + pyx2 + y 2 + R2


ŷ +

R
p

x2 + y 2 + R 2

 − 1 ẑ

With this equation, the non-linear mapping can be reversed using an interpolation routine.

(B.4)

132
In addition to the interpolation, the radiation at the edges of the Ewald sphere have propogated further than the radiation at the center. The intensity of the diffracted light on the dector
should be corrected as follows:
Iscaled (x, y, z) =
x2 + y 2
1+
I0 (x, y, z)
R2

(B.5)

where I0 is the raw recorded diffraction pattern.

B.3

Tilted Plane Correction
Thus far we have considered a sample plane parallel to the detector. For reflection geometry

imaging, unless the detector has a hole in it, the sample plane will be at some non-zero angle.
To describe the tilted sample, a rotation matrix is applied to ~q. In our experiment, the sample isrotated about the y-axis, so the following rotation matrix is used,sinα 
− cos α 0Ry (α) =  0

−1
0




− sin α 0 − cos α(B.6)

where α is the angle of rotation as depicted in Fig. B.1b. The rotated sample plane now lies in the(x00 , y, z 00 ) plane. The application of the rotation matrix to ~q yields~q(x00 , y, z 00 ) = Ry (α)~q(x, y, z)(B.7)~q(x00 , y, z 00 ) = (−qx cos α + qz sin α)x̂ − qy ŷ − (qx sin α + qz cos α)ẑ.

(B.8)

This results in a non-linear and asymmetrical mapping of the diffraction pattern onto the detector
plane as depicted in Fig. B.4. Again, using an interpolation routine, this non-linear mapping canbe re-sampled onto a linearly spaced gird.

133

Figure B.2: Low NA with Normal Incidence a) Side-view. The circles on the detector highlightthe same spatial frequency. b) Bird’s eye view. )Figure B.3: High NA with Normal Incidence a) Side-view. The circles on the detector highlightthe same spatial frequency. b) Bird’s eye view. )Figure B.4: High NA with Non-Normal Incidence a) Side-view. The circles on the detector
highlight the same spatial frequency. b) Bird’s eye view. )Appendix C

Near-Wavelength Resolution CDI in Reflection with EUV: supplemental figures

Figure C.1: Full-Field, high-contrast, ptychographic imaging with high-harmonic generation a) Amplitude and b) phase reconstructions using ptychography. c) An SEM image forcomparison. A zoom-in of the d) amplitude and e) phase of ptychographic reconstruction. The
zoom-in area is enclosed by the black rectangle in (c). g) The corresponding SEM zoom-in. h) AFM
image in the same zoom-in region. The retrieved f) amplitude and i) phase of the probe. The whitecircles highlight dust contamination. The dashed rectangle is the area used for the calculation of
the Modulation Transfer Function. The area enclosed by the white rectangle is used in the AFM
comparison. The scale bar in (b) and (i) corresponds to 10 µm. The scale bar in (h) corresponds
to 1 µm. Figure adapted from Zhang, Gardner et al. [168].

135

Figure C.2:
Later Resolution Characterization a) Phase retrieval transfer function. b)
Relative modulation transfer function with an AFM image as the “true image. c) Power spectral
densities of the CDI and AFM image, as labeled. d) The location of the knife-edge tests shown in(e) and (f). The profile across the e) x-direction and f) y-direction (dashed lines). An error-function
is fitted to the profiles with R2 better than 0.99 (solid lines). Figure adapted from Zhang, Gardneret al. [168].

136

Figure C.3: Axial Resolution Characterization a) Histogram distributions of the height differences between the calculated height using the phase reconstruction and an AFM image. The top
panel, no filtering and compares (c) and (d) directly. Middle panel only compares trench features,(c) and (e). The bottom panel compares a smoothed version of the AFM image, (c) and (f). (b)Comparative profiles taken along the white dashed line in (d). The top panel is no filtering, (c) and(d), and the bottom panel compares (c) and (f). (c) The calculated height from the ptychographic
phase reconstruction. (d) The AFM image. (e) Only the trench features of the AFM image. (f) A
Gaussian blurred image of the AFM to match the resolution of the CDI reconstruction. The scalebar in (f) corresponds to 2 µm and is shared with (c) (e). Figure adapted from Zhang, Gardneret al. [168].

Appendix D

Sub-wavelength coherent imaging of periodic samples: supplemental figures

D.1

Full ptychographic reconstruction of the zone plate sample
The full ptychographic reconstruction, covering an area of 11.3 µm × 11.3 µm, is shownin Fig. D.1. Only the reconstruction using the novel MEP constraint is shown. Degraded zone
plate features are seen in the upper right quadrant, but this is not an artifact of the reconstruction
because the same degradation is seen in the scanning electron microscope image in the inset of Fig.
8.1.

Figure D.1: Full ptychographic image of the zone plate sample with MEP The full,complex, ptychographic image of the zone plate sample, with MEP, where a) is the intensity andb) is the phase. The area highlighted by the blue box in (a) is the region shown in Fig. 8.3 andFig. D.2. The 5µm scale bar in (b) is shared with (a).

138

D.2

Phase images with and without the MEP constraint
Phase images, corresponding to the intensity images shown in Figs. 8.3b,c, are displayed inFig. D.2. The phase image without the MEP constraint, Fig. D.2b, suffers from artifacts such as
ringing and striping compared to the MEP reconstruction, shown in Fig. D.2a, where the phase of
the PMMA is smooth and continuous. In between the PMMA features, there are discontinues in
the phase image corresponding phase wrapping.

Figure D.2: Phase images of the zone plate sample Phase images of the zone plate sample(a) with the MEP constraint and b) without MEP. The 2µm scale bar in (a) is shared with (b).

139

D.3

Random Initial Probe Guess Simulations
As long as the diffraction patterns are properly sampled, no information about the probe isneeded for the MEP algorithm to converge. On the other hand, without the MEP constraint, thealgorithm will not converge using random probe guesses.

Figure D.3: Random Initial Probe Guess Simulation Results The MEP constrained ptychography algorithm is able to converge with random probe guesses. Without the constraint, thealgorithm did not converge.

140

D.4

White Gaussian Noise Simulations
Additive white Gaussian noise is added to the data at 100 dB signal-to-noise (SNR) and 50 dB

SNR. The ptychography algorithm with the MEP constraint converges to a lower root-mean-square(RMS) error in both cases.

Figure D.4: White Gaussian Noise Simulations The MEP constrained ptychography algorithm
reaches a lower error than the unconstrained algorithm