CHESS &CESRScience at the Hard X-ray Diffraction
Limit: XDL-2011 Workshops Summary

CLASSE

Sol M. Gruner
Director, Cornell High Energy Synchrotron Source (CHESS)& Cornell University Physics Dept.
smg26@cornell.edu

Synchrotron
Tunnel• Cornell ERL Context• XDL-2011 Workshops

ERL Phase 1
Linac

ERL
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CLASSE

Layout of Cornell ERL
a 5 GeV, 100 mA, hard X-ray light source

ERL main linac: 5 GeV, 100 mA
with energy recovery

CESR
ERL injector

Undulators
and X-ray
beam lines

Beam Stopslide credit: M. Liepe

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ERL Specifications1
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CLASSE

Energy range: tunable, VUV to hard x-ray (30 eV to 100 keV)
Spectral brightness: 1022 to 1023 x-rays/s/mr2/mm2/0.1%bw
Highly Coherent Source: 60% at 10 keV in Hi-coherence mode
2 micron diameter round electron beam facilitates nanoprobe
imaging
Short pulse: ~50 fsec
Hi-flux mode: 100 mA, 25m undulators w/many short periods
Tiny electron energy spread (2x10-4) for 1000 period undulators.
Many simultaneously operating ID stations
Very flexible operating modes, controlled by injector laser.
Can run with non-recovered interleaved pulses (+ fast kicker)
High repetition rate avoids local sample heating, allow multiple
exposures of a sample. Very important for materials science.

The breadth of science and technology enabled is huge. ERL will
be a resource for many sciences, especially materials science.
1. Different modes are not all simultaneous

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Cornell ERL Project Timeline

CLASSE

1999: Maury Tigner suggests a coherent hard x-ray ERL light source is now feasible.
2000: 1st X-ray Science Workshop for an ERL @ CU
2001: Cornell and JLab groups put out ERL “white” paper
2005: Phase Ia: $18M- NSF, 5-yr R&D on injector, linac modules, machine issues.
2006: Six x-ray Science Workshops for an Energy Recovery Linac @ CU
2006: Conceptual engineering studies for Phase II ($12M NY State + CU support)
2008: NSF Light Source Panel recommends that the NSF should build & steward a coherent lightsource (Venky report, www.nsf.gov/mps/dmr/LSPanel_FinalRPT_wCorrections9_15_08.pdf )2009: ERL09: 45th ICFA Beam Dynamics Workshop on Energy Recovery Linacs, June 8-12, 2009at Cornell University
2010: Phase Ib: Continued R&D. $32M (NSF, 4 year duration).
ERL civil construction design study completed.
2011: April, ERL technical design report completed & passed to chosen reviewers.
May, ERL draft Environmental Impact Statement ready for submission
June, XDL-2011 with 6 X-ray Science workshops at Cornell
October, ERL-2011, 50th ICFA Advanced Beam Dynamics Workshop at KEK
November, Cornell announces emittance and SRF cavity milestones????: Phase II: Transition to a 5 GeV ERL x-ray facility as NSF MREFC upgrade to CHESS as fast as
possible (~5 year build).

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Cornell ERL Civil Engineering Study

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CLASSE

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ERL R&D at Cornell

CLASSE

Outline of HZB test ERL, one of several proposed/approved ERL test facilities

Many R&D Challenges. Foremost:• Can an injector be made to deliver required emittance?
• Can the injector operate with acceptable current and lifetime?
• Can the main linac operate with acceptable Q0 and HOM
performance at 100 mA?
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Verification of ERL Beam Production:
Cornell Injector Test Facility

CLASSE• Key parameter for ERL• Improvements in the source immediately translate to a better
performance of the entire facility• Source development at Cornell– 5-15 MeV injector– New 500kV DC gun + beamline

dump

diagnostics

SC injector

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Milestones at Cornell’s injector

CLASSE

Peak DC-beam current: 25mA (meets high coherence mode spec)
Peak bunched-beam current: 25mA with GaAs / 20mA with CsK2Sb for 8h
Peak charge per bunch: 200pC (more than needed)
Typical bunch length: 2ps (up to spec)
Smallest normalized emittance after injector at 80pC: 0.8 mm mradwith normalized bunch core emittance : 0.3 mm mrad
For this gun, 0.5 mm mrad is theoretical limit !
Emittances scale in linac as 1/γ. At 5 GeV, 0.3 mm mrad → 30 pm.
20pC: 0.4 mm mrad; 0.15 mm mrad core
Largest SRF-injector cavity Q0: 1.e10 (of 2.e10 required)
Largest injector-coupler power: 60kW (of 100kW required)
Largest SRF-cavity voltage: 13MV/m (up to spec)

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ERL cavity fabrication and measurement

CLASSE

Q vs. E for 1st prototype Cornell ERL cavity
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Towards Fourier-limited X-ray Science
Shin-ichi Adachi, Photon Factory, KEK & PREST, JST
Workshop 3: Ultrafast Science with “Tickle and Probe”

A continuous sequence of ultralow emittance multi-GeV electron bunches and a lowloss optical cavity constructed from high-reflectivity Bragg crystals can create an Xray FEL Oscillator (XFELO). The x-ray beam from an XFELO would be Fourier transform
limited, have tunable wavelength, and
X-ray Beam Properties
the peak power would be small enoughPhotons/pulse
109
to not adiabatically damage samples.
The beam will have an average spectral
Rep rate
1-100 MHzbrightness 103-105 x greater than
-6
dE/E
10
available on existing or planned sources.
τ

CLASSE

K.-J. Kim

1 ps

K.-J. Kim, et al., Phys. Rev. Lett. 100 (24) (2008).

The X-ray beams produced by an XFELO would be fully Fourier-limited, upgrading existing
techniques or enabling novel ones such as nonlinear X-ray optics, inelastic scattering, twophoton correlation spectroscopy, and transient grating spectroscopy. For example, the meVenergy resolution would enable inelastic scattering studies of thermally generated excitations
in small samples.
Y. Shvyd’ko
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Science at the Hard X-ray
Diffraction Limit (XDL-2011)

CLASSE• Series of 6 workshops at
Cornell in June, 2011
• Co-sponsored by SSRL,
DESY, Photon Factory;
funded by NSF & DOE• Lots of interest andexcitement• Lots of ideas for greatscience enabled bycontinuous duty, coherent xray sources (ERLs & USRs)• 488 participants
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Workshop Titles & Organizers

CLASSE

http://erl.chess.cornell.edu/gatherings/2011_Workshops/index.htm

WS3 cover graphic

WS6 covergraphic

WS1: Diffraction Microscopy, Holography and Ptychography using Coherent Beams
Organizers: Janos Kirz (Lawrence Berkeley National Lab), Qun Shen (National Synchrotron Light Source II), &Darren Dale (Cornell University)
WS2: Biomolecular Structure from Nanocrystals and Diffuse Scattering
Organizers: Ed Lattman (Hauptmann-Woodward Medical Research Inst.), Mavis Agbandje-McKenna (University of
Florida), Keith Moffat (University of Chicago), & Sol Gruner (Cornell University)
WS3: Ultra-fast Science with “Tickle and Probe”
Organizers: Robert Schoenlein (Lawrence Berkeley National Laboratory), Brian Stephenson (Argonne National
Laboratory), Eric Dufresne (Advanced Photon Source) & Joel Brock (Cornell University)
WS4: High-pressure Science at the Edge of Feasibility
Organizers: Russell J. Hemley (Carnegie Institution of Washington), Neil Ashcroft (Cornell University), Roald
Hoffmann (Cornell University), John Parise (SUNY Stony Brook), & Zhongwu Wang (Cornell University)
WS5: Materials Science with Coherent Nanobeams at the Edge of Feasibility
Organizers: Christian Riekel (European Synchrotron Radiation Facility), Simon Billinge (Columbia University),
Kenneth Evans-Lutterodt (Brookhaven National Laboratory), & Detlef Smilgies (Cornell University)
WS6: Frontier Science with X-ray Correlation Spectroscopies using Continuous Sources
Organizers: Mark Sutton (McGill University), Simon Mochrie (Yale University), & Arthur Woll (Cornell U.)

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Materials Overview
Simon Billinge (Columbia), Paul Evans (U of Wisconsin)& Reinhard Boehler (Carnegie Institution of Washington)

CLASSE“Advances in materials science lie on the critical path of many technologicalsolutions to mankind's most pressing problems, such as sustainable energy,
environmental remediation and health. Increasingly we seek materials that havedirected functionalities, in analogy with enzymes in biological systems, that can bebuilt up into more complicated devices. This necessitates the study of materials
of increasing complexity, for example, larger unit cells, more complicatedcompositions, heterostructures on the nanometer and micrometer length-scales,and structural modifications on the nanoscale. Nanostructured materials are at
the heart of many of these proposed technologies.”, Simon Billinge

Coherent diffraction imaging of electronic
textures in correlated materials.
Information is available on nanometerspatial scale. Josh Turner et al., New J.
Phys. 10 (2008) 053023.

“These emerging hard x-ray sources can be focused to small spot sizes, atwhich they can provide high-resolution structural information via either
diffractive imaging or scanning techniques. The fs to ps bunch duration of theelectron bunches at these sources inherently allows such probes to provide
time resolution simultaneously. Key examples of the scientific impact of thesedevelopments will arise in the study of both reversible and irreversible materials
processes. The scientific needs for these probes arises in the study of fundamental
excitations, GHz mechanics, dynamics in magnetic and spintronic devices, anddynamics and extreme conditions in complex oxides, etc.”, Paul Evans“Melting at high pressure is of fundamental interest and plays a key role in estimates on temperatures in planetaryinteriors and on the dynamics of dynamos creating magnetic fields and dynamics of motion in planetary mantles and plate
tectonics. Melting temperatures of both metals and silicates/oxides measured statically in laser-heated diamond cells
are in serious disagreement with those obtained from shock experiments for transition metals. Diffraction
measurements on a millisecond resolved time sequence could resolve this issue to follow the structural evolution
during the melting-freezing event.” Reinhard Boehler
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Materials Processing
Ross Harder, Argonne National Lab
CLASSEWorkshop 1: Diffraction Microscopy, Holography and Ptychography using Coherent Beams
Since the mid 1950’s researchers have only been able tospeculate on the microscopic mechanisms of the mostfundamental aspects of grain nucleation and defectformation. Annealing twins, which play a critical role in themechanical strength of FCC metals, are seen to emanatefrom grain boundaries during growth. Yet very little is
known about the mechanisms through which they format specific locations on grain boundaries.
Coherent diffraction imaging in the Bragg geometry offers aunique capability to study the mechanisms of grain growth on
the nanoscale. Unique to Bragg CDI is an ability to study
a single crystalline domain, buried in a thickpolycrystalline sample, with nanometer spatial
resolution. Because the method exploits the coherent
scattering in the vicinity of Bragg peaks to obtain images ofthe sample, it can also be used to map strain in the crystalline
lattice, which can be caused by defects and dislocations.

Top: Coherent Bragg diffraction from a nanocrystal [Pfeifer, Nature,442, 63]. Bottom: Reconstructed amplitude and phase of a single ZnO
nanorod for six Bragg reflections [Newton, Nature Materials, 9, 120]

Using the two to three orders of magnitude greater coherent
hard x-ray flux afforded by an ERL or USR source, we will beable to image the evolution of such materials properties
on time scales of minutes at sub ten nanometer
resolution.

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3-D Nanodiffraction to Improve Polycrystalline Materials
Gene Ice, Oak Ridge National Laboratory
Workshop 5: Materials Science with Coherent Nanobeams at the Edge of Feasibility

CLASSE

Improving polycrystalline materials, such as metals
and ceramics, is a fundamental goal of materials
science. Materials behavior is dominated by defects andheterogeneities on micron and submicron length scales,
information that is hard to extract from ensemble
averages. X-ray methods are particularly importantbecause they can nondestructively interrogate local strain,
structure and texture of imbedded volumes to follow how
real materials respond to loads and processing variables.
This information has simply not been available.

Schematic multi-probe 3-D nanoprobe station (Courtesy of G. Ice)

Two important, recently developed x-ray approaches todiffraction mapping are differential aperture
microscopy, and 3-D diffraction microscopy. These
techniques are severely limited by scan times atexisting x-ray sources.

ERLs/USRs will have two huge impacts on differential aperture microscopy: (1) The high focused beam intensity will allow
rapid measurements, and (2) the small beam size will allow for advanced achromatic optics with diffraction limited beam sizes
and useful working distances. For example, with fly-scan methods and feasible detectors, it will be possible to map volumes
with 2x106 volume elements/ hour. This will enable unprecedented visualization of materials structure and behavior inminutes, instead of days.
Beyond existing methods, the instrumentation developed for differential aperture microscopy has implications for coherent
imaging of important materials. Already coherent imaging has achieved spatial resolution of 2 nm. Given the proposedbrilliance of ERLs and USRs, it will be possible to extend the differential-aperture microscopy into the coherent regime to gain
spatial resolution at far smaller length scales than possible today.
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Dynamics of soft matter & complex fluids
Y. Shinohara1, W. Burghardt2, A. Fluerasu3, S. Mochrie4 , L. Lurio5
Workshop 6: X-ray Correlation Spectroscopy using continuous beams

Nonlinear viscoelasticity
Uniform shear

Shear banding

CLASSE

Many engineered and biological soft materials, suchas polymers, colloids, emulsions, gels, etc., exhibit
important but poorly understood behavior in nonequilibrium conditions, such as non-linear viscosity
during flow (left). For example, although colloidal
particles are often added to rubber to manipulate
performance, the affect of such additives on
elasticity and viscosity is difficult to predict.

Colloidal aggregates in soft-matter The origins of such behavior involve molecular-scale
fluctuations on length scales of 10-1000 nm and 10
6-10-2 second time scales.

XPCS can directly measure these fluctuations,but such length and time scales require 2-3
orders of magnitude more coherence flux.
ERL/USR sources should make suchmeasurements routine, with potential impacts in
100nm
many areas of application, such as improved tire
1Department of Advanced Materials Science, University of Tokyo
performance.
2Department of Chemical and Biological Engineering,

3NSLS-II, Brookhaven National Laboratory

Northwestern University

4Department of Physics, Yale University
5Department of Physics, Northern Illinois University

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Atomic Diffusion
Bogdon Sepiol, Department of Condensed Systems, University of Vienna
Workshop 6: X-ray Correlation Spectroscopy using continuous beams

Different jumpmechanisms

CLASSE

Atomic diffusion is critical to materials
synthesis and stability, and thus
dictates the behavior of much of thematerial world. Yet, it is difficult tomeasure directly, and imperfectly
characterized in most systems of interest.
XPCS provides direction-specificsensitivity to atomic diffusion in bulk
materials, but requires measurement offluctuations in weak, diffuse scattering
between Bragg Peaks.
Demonstration experiments at ESRF
employed count rates of

1 count per 10 minutes per pixel!
Diffuse Scatteringfrom a bulk crystal

ERL/USRs would increase count rates
by upwards of 3 orders of magnitude,
rendering such measurements routine,
and allow different jump mechanisms
to be distinguished.
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Nanoscale Phase Separation in Correlated Oxides
Oleg Shpyrko, University of California at San Diego
CLASSEWorkshop 1: Diffraction Microscopy, Holography and Ptychography using Coherent Beams
Strongly correlated systems often feature competing spin,
charge, orbital and lattice degrees of freedom, which result in
spontaneous emergence of nanoscale inhomogeneities, which
can strongly influence material properties. These domains
typically occur as a result of competition between phaseseparation and strong correlations. However, it is not yet clear
whether domain structure arises primarily from these interactions,or if crystalline imperfections – such as lattice strain, defects orinhomogeneous distribution of dopants – may strongly influence
formation of textured domain patterns.

Examples of nanoscale inhomogeneities in a variety of strongly
correlated systems: (A) Scanning Tunneling Spectroscopy of theinhomogeneous superconducting gap distribution as well as stripe(or checkerboard) patterns in underdoped high-Tc superconductors[Tranquada, Nature, 429, 534; Dagatto, Science, 271, 618] (B)Phase separation in Colossal Magnetoresistive (CMR) Manganites[Mori, Nature, 392, 473; Mathur, Physics Today, Jan 2003, p26]
(C) Charge-Density Wave [Shpyrko, Nature, 447, 68] and SpinDensity Wave (inset) [Evans, Science, 295, 1042] domains in
Chromium; (D) Coexistence of Conducting and Insulating domains
in VO2 at the onset of the Metal-Insulator Transition [Qazilbash,
Science, 318, 1750]

Resonant microdiffraction and lens-less imaging can beused to study spin, charge, lattice and orbital degrees of
freedom in correlated electron systems, as well as strain anddefects, with nanometer-scale resolution. These types of
microscopy studies will answer many fundamental questions
about how electronic correlations emerge, what role crystalline
disorder plays in their formation, and the interplay between these
degrees of freedom, which results in complex competition andcoexistence between various ground states.
The high coherent flux produced by an USR/ERL will make itpossible to study the dynamics of this competition attimescales 100 to even 10,000 times faster than at thirdgeneration sources. Imaging structures will be 100 times
faster than at third generation sources, such that nanoscale
resolution could become routinely accessible.
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Steady-state, non-equilibrium surface dynamics
Michael Pierce1, Karl Ludwig2
Workshop 6: X-ray Photon Correlation Spectroscopy (XPCS) using continuous beams

Sputter-induced pattern formation on Si

Diffuse scattering rises,
then reaches steady stateAu(001) in HClO4

CLASSE

Surface processing is ubiquitous in industry, yet is often
poorly understood due to inherent challenges ofcharacterizing non-equilibrium processes at atomic lengthscales and in challenging process environments. In situ
XPCS allows direct observation of surface
fluctuations at well-defined time and length scales,
offering a powerful new approach to the study of suchprocesses.
During sputter-induced pattern formation on silicon(upper left), an initially smooth surface reaches a
dynamical steady state, in which the morphology, andtherefore the diffuse scattering pattern, remains
statistically constant despite the fact that it continues to
evolve. Similarly, Electrochemical processes (lower left)
are of critical importance in a broad range of fields, yetremain challenging to study.

L (rlu)In each case, in situ XPCS offers the unprecedented
possibility of continued observation of suchprocesses even after the morphology reaches its
steady state, providing new, detailed insight into
kinetic processes, yet require the 102-103 times
greater brilliance of an ERL/USR to become practical.

Time (sec)

1Department of Physics, Rochester Institute of Technology
2Department of Physics, Boston University

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Nanotomography for Materials under Extreme Conditions
Wendy Mao, Stanford University
Workshop 5: Materials Science with Coherent Nanobeams at the Edge of Feasibility

laser

nanoXCTBe gasket

samplethermalinsulation
layersdiamond anvil

6 GPa
2073 K

5 m

Fe + 10wt% S spheres within olivine matrix

CLASSEHigh pressure research is a rapidly changing and expanding field,
both with regards to materials of interest as well as x-ray techniques.
The latter development is driven by the emergence of very highbrilliance x-ray sources. Of particular interest is combining
nanobeam x-ray computed tomography (nanoXCT) with diamondanvil cell technology (upper left figure). This enables the study ofmulti-component materials under high pressure and at hightemperature, as shown in the lower left figure. nanoXCT contrast
mechanisms include absorption, scattering, and element-specificfluorescence, but also inelastic scattering and x-ray Raman
scattering are of high interest to be able to distinguish between
different phases and their shape and volume changes under
extreme conditions.
Tomography facilitates characterization of texture and shape ofmulti-phase assemblages, the precise determination of the volume of
amorphous materials, density of light-element phases and themorphology of nanomaterials. In addition the multiprobe approach
will make it possible to study chemical reactions, defects, anddiffusion of materials under high pressure and at high temperature.
An ERL or USR will enable high-flux nanobeams at high-energy,
enabling high-resolution 3D imaging on a fast timescale that will
enable diffusion and deformation processes to be studied in realtime. With the newly acquired capability of studying complex
materials under extreme conditions as well as the advent of new
high-brilliance x-ray sources, high-pressure research is poised towrite a new chapter.
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Synchrotron techniques: x-ray tomography and imaging throughdiamond anvil cells
CLASSE
Wenge Yang -- HPSynC & Geophysical Laboratory of Carnegie Institution of Washington
Workshop 4: High Pressure Science at the Edge of Feasibility

Nanofocused x-ray beams are being used to: understand phase & grain boundary evolution,measure density in-situ, study structure of confined liquids & non-crystalline solids, andmonitor strain as a function of pressure.
Coherent diffraction imaging (CDI) of nanoscale strain has wide
application for understanding nanomaterials under extreme pressure& temperature, and during deformation or chemical processing.
X-ray methods are especially suited for in-situ measurement for
example inside a diamond anvil cell (DAC).

CDI near (111) reflection of 200nm gold particle
M.A. Pfeifer,et.al. Nature (2006). Lattice

Nanoscale materials often exhibit unusual strength so it is important
to examine them under stresses that lead to breakdown. X-ray CDI
can also be used to study pattern formation in materials synthesis, forexample to understand growth limitations associated with self-assembly inthe presence of surfactants.
ERL beams will have unprecedented transverse coherence and flux
up to 60KeV, and the small round source is ideal for nanometer
focusing and for matching horizontal & vertical coherence lengths.
Upper left illustration: CDI experiment and representative data.
Lower left: Phase retrieval methods can produce 3-dimensionalstrain maps - color represents atomic scale lattice strain along
specific directions resulting from pressures & surface truncation.

CDI reconstruction yields lattice strain map ofgold under pressure W.Yang, (early results).

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Time and momentum domain inelastic scattering from phonons
David A. Reis, SLAC National Accelerator Laboratory
Workshop 3: Ultra-fast Science with “Tickle and Probe”

CLASSEA high-repetition-rate, femtosecond, hard x-ray source would be uniquely suited for studying electronic andvibrational dynamics with atomic-scale temporal and spatial resolution. For example, such a source
would allow one to perform momentum resolved inelastic scattering in the time-domain, which isparticularly well suited for studying phonon dynamics: phonon-phonon and electron-phonon coupling.
A striking example is the efficiency of photovoltaics, which is often limited byenergy loss from the photo-excited electrons to phonons, such that the photon
energy above the band-gap is lost to heat. In this experiment, an opticallaser pulse is used to excite the sample repetitively. A variable time-delayed
hard x-ray probe is used to scatter from the excited volume. The timeresolved diffuse scattering is captured on an area detector. To first order,
time-dependent changes in the intensity of a given pixel reflect changes in the
population of phonons of a particular q. Thus, one can follow the
nonequilibrium phonon population from the initial emission from the hot
electrons through the subsequent anharmonic decay until the lattice
thermalizes.
Recent demonstration experiments at a 3rd generation source on
photoexcited InP show that the phonon population remains out of equilibrium
for hundreds of picoseconds to nanoseconds. However, high optical driving
power is necessary to massively populate the phonons and the critical earlytime regime is inaccessible. The ERL/USR would provide both the shortpulses and the required flux.

M. Trigo, J. Chen, V.H. Vishwanath,
Y.M. Sheu, T. Graber, R. Henning,and D.A. Reis, Imaging nonequilibrium
atomic vibrations with x-ray diffuse
scattering. Physical Review B, 2010.
82(23): p. 235205.

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Tracking energy flow in light-harvesting antenna-proteins
Ed Castner, Rutgers
Workshop 3: Ultra-fast Science with “Tickle and Probe”

CLASSE

Biomimetic researchers copy or incorporate biologicalprocesses or components into engineered materials,
processes, or devices. For example, light-harvesting antennaproteins collect solar energy and efficiently transport the resulting
electron-hole pair to a photosynthetic reaction center where
chemical synthesis occurs. The ability of light harvesting
molecules to efficiently guide energy makes them intriguing
candidates for components in nanofabricated photonic devices.
[We] report the first observation of long-range transport of
excitation energy within a biomimetic molecular nanoarray
constructed from LH2 antenna complexes from Rhodobacter
sphaeroides.

The electronic excitations travel up to 50nm and are believed tolast for 100’s of ps in an individual protein. In the example on
the left, an nanofabricated array of antenna-proteins transports
the excitation over microns.

Escalante, et al., Nano Letters, 2010. 10(4): p. 1450-1457

Resonant Inelastic X-ray
Scattering (RIXS) measurements
provide access to the unoccupied
electronic structure information
present in XAS and correlate it withthe occupied electronic structure
information present in XES
measurements, producing acomplete description of valence
excitations.

Temporally (ps) and spatially (10 nm) resolved RIXS
could map the migration of the electronic excitation
following (optical) photoexcitation. The energy
tunability, high spectral brightness, few nm x-ray spot
sizes, and high repetition rate, sub-ps pulses of the
ERL/USR enable this type of measurement.

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Static and Dynamic heating of Materials
Reinhard Boehler, Carnegie Institute of Washington
XDL Workshop 4: High Pressure Science at the Edge of Feasibility

CLASSEAn understanding of melting phenomena at high pressure is of fundamental interest, critical for
estimating planetary interior temperature, understanding magnetic fields and material transport within planetarymantels and tectonic plates. Yet serious disagreement exists
Diamond cell
(as indicated in the lower figure) when comparing the melting
pulsed laser
phase diagram, of metals & silicate oxides, measured in aheating &laser-heated DAC and by shock driven methods. Systematic
below melting
melting measurements, at extreme temperature & pressure
curves fromhave not been possible to do using synchrotron radiation, but
DAC & shock
recent SEM studies indicate that experimental problems canexperiments.
be circumvented in millisecond x-ray measurements. This
would be accomplished if msec. pulse-laser heating ofsamples inside the DAC were monitored, in time, by
sequential, microsecond x-ray diffraction study. The flux
available in ERL pulses would help address the possible
existence of a plastic-like state before melting of bcc metals
like Ta, W & Mo. Through focusing of extremely bright ERL
beams one could measure local stress-strain behavior acrossthe pulse-laser heated sample. This would help provide
estimates of sound velocity that will lead to better
understanding of the Earth’s core.

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Understanding Planetary Interiors with an ERL
J.M. Jackson & D. Zhang, Caltech
Workshop 4: High Pressure Science at the Edge of Feasibility

CLASSEAn understanding of the dynamics & composition of planetary interiors will lead to new insights about thesolar system and better interpretation of seismic data collected here on earth. This depends on
knowledge of material characteristics such as melt viscosity,
elastic constants, sound velocity and thermodynamic
parameters of liquid-iron alloys and other earth materials, atpressures in excess of 100GPa and temperatures greaterthan 1000K.
The ERL will deliver 100 times the flux/unit energy/squaremicron of existing storage rings or those under construction, inthe energy range of interest here. This will enable new classesof experiments, like momentum-resolved inelastic scattering(IXS) on individual grains within assemblages inside diamondanvil cells (DAC).
Figure illustrates why knowledge of p-,s-wave sound speed andmaterial properties through the core, mantle and interface
region is essential for seismic interpretation.

X-ray stimulated nuclear resonance measurement of acoustic
vibrations yield sound speed, IXS reveals anisotropy &phonon dispersion, melting & structural phases are identified
by diffraction, and emission & absorption spectroscopies
provide chemical information. The ERL will enable delivery of
unprecedented sub 100nm focused beams for: selection andimaging of individual grains, measuring diffusion constants at
microsecond time scales, and revealing liquid dynamics in thepico- to nano-second range.

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Determine 3D Nanomorphology for Improving Organic Solar Cells
CLASSE

Harald Ade, North Carolina State University
Workshop 1: Diffraction Microscopy, Holography and Ptychography using Coherent Beams
Light

Solution-processed organic solar cells are attractive as low-cost
photovoltaic technology. They can be spin-coated or printed like anewspaper or ink-jet coated onto flexible substrates of plastic or glass.
Currently most designs are based on bulk heterojunction (BHJ) structures of
100 to 200 nm thickness. Even a two-phase description is idealistic. A
complex morphology of at least three phases might have to be considered.
To be efficient, the inter-digitated electrodes must be only
separated by 10 to 30 nm.
OO

To establish full control, one needs to control the average domain size, domain size distribution,
domain purity and domain interface widths. For each of these novel materials systems, themiscibility, morphology and domain purity, connectivity of domains, crystallinity, phase andinterface properties need to be measured in order to understand device performance deeply andrationally seek processing and materials improvements.
Characterization of 3D structure of organic blends with ~10 nm resolution poses a key technicalchallenge. High-resolution hard x-ray scattering, electron tomography and TEM have only
limited electron density contrast for these polymer/polymer blends, limiting the use of
conventional tools for these materials. A new suite of analysis tools such as 3D resonant
ptychography or holography with compositional sensitivity are required.
These forms of coherent imaging require bright sources and would be well matched to an
Energy Recovery Linac. Ideally, multiple energies near the carbon K 1s absorption edge (i.e.
260-320 eV) are utilized to provide maximum compositional sensitivity. Thus, advanced
imaging tools enabled by an ERL would be able to make tremendous contributions toimproving Organic Solar Cells.

PC71BM
OCH3

O

PC61BM
*

N

N

*

n

PFB
R

R

*

*
S

S

F8TBT

n
N

N
S

*

S

*

n

P3HT
PBTTT

C14H29

S

*
S

S

*

S

C14H29n

P(NDI2OD-T2)
285
290
Photon Energy [eV]26
KEK-IMSS 6 Dec 2011

Speed Limits for Ferroelectric/Multiferroic Switching
Aaron M. Lindenberg, SLAC National Accelerator Laboratory
Workshop 3: Ultra-fast Science with “Tickle and Probe”

CLASSE

Complex-oxide multiferroic materials are promising candidates for advanced technological applications. A high-repetition-rate,
ultra-fast, hard x-ray source will provide the capability to study the speed limits to switching in these materials.
Similar to ferromagnets, ferroelectrics minimize
their energy by breaking into antiphase domains,
frequently with a characteristic length scale. Short
range ordering of these domains produces diffuse
x-ray scattering features in addition to the sharp
Bragg peaks from the lattice.
The ferroelectric stripe phase of PbTiO3 can by destroyed or enhanced by an
ultra-fast optical pulse with rapid relaxation on few nanosecond time-scales,enabling high-rep-rate experiments of ultra-fast switching and nucleation
dynamics.
T=430C ferroelectric phase (PbTiO3 on DyScO3)• Reversible optically‐induced switching from ferroelectric to paraelectricphase at fluences <100 μJ/cm2• Recovers on few hundred picosecond time scale
The flux of the ERL/USR will enable ultra-fast, high-repetition rate, pump-probe
studies with much less intense pump pulses. One expects flux increases of 104
relative to existing slicing and low-alpha sources

27
KEK-IMSS 6 Dec 2011

nanoXRF and nanoXANES in Art Conservation
Jennifer Mass, U Delaware and Winterthur Museum
Workshop 5: Materials Science with Coherent Nanobeams at the Edge of Feasibility

CLASSE

Preserving the cultural heritage of mankind has become a major
challenge in art conservation. This shall be illustrated by color alterations
in Impressionist and Early Modern Art masterpieces. Degradation ofpigments by either oxidation or reduction has led to fading and color shifts
all the way to catastrophic failure in the works of van Gogh, Matisse, Manet,
Seurat, and Picasso.

Color alteration in a Seurat painting,as seen in the cross section of a paint chip

Photo-induced degradation is a surface phenomenon, often occurring in
only the top 1-5 microns of the paint layer, and the photo-degradation
products are often minor phases within this alteration layer. The
preservation of the icons of early modern art hinges on the spatiallyresolved atomic and molecular characterization of these minuteheterogeneous alteration layers, an analytical challenge requiring nondestructive chemical imaging with at least nanogram sensitivity. New
rapid, high resolution, and highly sensitive chemical imaging tools for the
inorganic and organic components of the disfiguring degradation layers areneeded.

From merely analyzing the damage mechanisms, efforts in art conservation aim to detect damage in its early stages andprevent further degradation. Analyzing the surface pigment layers requires confocal XRF and XANES microscopy withnanoscale resolution. In order to keep up with the large amount of endangered artifacts, fast scanning and analysis
methods will be mandatory.
An ERL will have major impact on x-ray confocal microscopy. So far achieved 3D resolution ranges from 1 micron toseveral microns, i.e. pigments could only be imaged as a whole or as an ensemble. Only the unprecedented average
brilliance of an ERL will make such an highly efficient chemical nanoprobe feasible.

28
KEK-IMSS 6 Dec 2011

Probing Organic Microstructures with Spatially Resolved
NanoGISAXS

CLASSE

Stephan V. Roth, DESY
Workshop 5: Materials Science with Coherent Nanobeams at the Edge of Feasibility
droplet drying
As nanotechnology and organic electronics move towards device

PolymericNanochannels
 Organic circuits
 Bioanalytical assays

P. Müller-Buschbaum et al.
APL 88, 083114 (2006)

applications and production, the new objects of study are smallorganic deposits on a substrate as microdrops (inkjet printing, offset
printing) or microwires (organic circuits). The new challenge is to study
the effects of new boundary conditions such as curved interfaces aswell as drying and processing kinetics. This requires probing such
structures on a submicron scale in-situ and in real-time. While first
nanoGISAXS has been demonstrated [Roth et al., Appl. Phys. Lett. 91(2007) 091915], much development remains to be done. Fast
scanning nanoGISAXS for real-time studies helps to stay one stepahead of the radiation damage.
These goals require a multiprobe approach combining various x-ray
detectors (area detectors, fluorescence detectors) and ancillary probes
such as optical microscopy, ellipsometry, or AFM. An imaging
ellipsometer was recently commissioned at MiNaX beamline of the
Petra III facility [Roth et al., J. Phys.: Condens. Matter 23 (2011)
254208]. nanoGISAXS can be combined with other methods such as
microtomography, using either the absorption or the scattering signal[Kuhlmann et al, Langmuir 25 (2009) 7241.], to retrieve 3D information.
The highly coherent nanobeams at an ERL or USR will facilitate areconstruction of the real space electron density via coherent
diffraction imaging, as demonstrated in first test experiments [Yefanov
et al, Appl. Phys. Lett. 94 (2009) 123104]. An ERL or USR will provide
the coherent flux for fast real-time studies. With the advent of new
brilliant sources, GISAXS with micro- and nanobeams is looking into abright future.
29
KEK-IMSS 6 Dec 2011Collective Coherent Control: Shaped THz Fields
Aaron M. Lindenberg, SLAC National Accelerator Laboratory
Workshop 3: Ultra-fast Science with “Tickle and Probe”

CLASSE

Ferroelectric materials are critical components in novel
electronic devices and have potential as storage
devices. Understanding the fundamental limits to theswitching mechanisms is critical to the development
process.
Goal is to explore ferroelectric switching by driving the soft
phonon modes which underlie ferro-electricity and study the
structural response with x-rays. One can drive the systemfrom the + polarization state to the – polarization state withthe appropriate THz pulse. The energy surface has a local
maximum at P=(0,0). By tailoring the THz pulse, one candrive the system through the saddle point and lower theenergy barrier to polarization switching.

T. Qi, T., et al. Physical Review Letters, 2009. 102(24): p.
247603.

In addition to providing high rep-rate, ultra-short x-ray
pulses, ultrashort electron bunches may enable thegeneration of the appropriate THz pump pulse sequence
directly from the electron beam, eliminating timing
jitter. Electron bunches in the required 10-100 fs regime will
be available from ERL and USR sources. The 10-100 ps
pulses from current storage rings are too long to create theTHz pulses.
30
KEK-IMSS 6 Dec 2011

Overview: Outstanding problems in biological science
Ilme Schlichting (Max Planck Inst. Heidelberg) & Mavis Agbandje-McKenna (Univ. Florida)
Workshop 2: Biomolecular Structure from Nanocrystals and Diffuse Scattering

CLASSEThe dream of the structural biologist is to visualize cellularcomponents (e.g., macromolecules, complexes and organelles) athigh, 3-D spatial and temporal resolution in defined functional states.
This information is vital to understand function of cellular processes,
and informs on cellular regulation, which helps the development ofdisease treatment strategies.
Many cellular components have poorly understood structures, including
weakly bound complexes, membrane proteins, transient intermediates(including catalysis and folding), chromatin, the nuclear pore complex, theGolgi apparatus, membrane fusion pores, many viruses – the list goes on.
Conventional x-ray methods are limited by the need for large crystals,
exposure times that are longer than the process being studied, andradiation damage. The intense, temporally short, coherent
nanobeams from ERLs and USRs open vast new areas for study:
Nanobeams enable structural determination from crystals that are only
practically available in the submicron range. Nanobeams also enable timeresolved solution scattering studies of transient structures in fluid jets.
Coherent diffraction methods yield structural information on non-periodic
cellular systems on nanometer length scales. Intense subpicosecond
pulses provide time-resolved snapshots of triggerable proteins. The
high brilliance enables rapid 3-D ptychographical methods on hierarchicalmaterials (e.g., bone, teeth, shells).
31
KEK-IMSS 6 Dec 2011

Time-resolved structure of macromolecular folding
Christian Riekel (ESRF), and Lois Pollack (Cornell Univ.)
Workshop 5: Materials science with coherent nanobeams at the edge of feasibility

CLASSE

Most cellular chemistry occurs in solution, and often involves
dramatic and rapid changes in structure. Phenomena that are notunderstood, but central to cellular function include folding ofproteins and RNA, multimeric complex association anddisassociation upon ligand binding, and alteration in
macromolecular structure upon changes in the surrounding
solution chemistry.

Lithographically fabricated lamellar
flow micromixer used to study
macromolecular folding. See Russell
et al., PNAS, 99 (2002) 4266.

Merging inkjet microdrops. Rita Graceffa,
PhD thesis, Grenoble (2010)

Spectroscopy is of limited use in determining global structure. But
small and Wide Angle X-ray Scattering (SAXS/WAXS) can provide
this information when coupled with methods to rapidly initiate
reactions and acquire x-ray data. The recent development oflamellar flow mixers and inkjet drop mixers enable rapid
reaction initiation by solution mixing down to tens of
microseconds.
The experiments are challenging because of the micron-sizedwidths of sample involved and the need to gather the scattering
data in very short periods of time. In the case of lamellar flow
mixers, reduction of background from the surrounding fluid
requires a beam that is on the order of the jet width, which is
microns for the fastest time scales. In the case of the inkjet
mixers, data must be acquired on time scales that are fastcompared to the movement of the droplet. Both considerations
require the intense microbeams possible with ERLs and
USRs.
32
KEK-IMSS 6 Dec 2011

New opportunities in time-resolved solution scattering of proteins
Phillip Anfinrud, NIH
Workshop 2: Biomolecular Structure from Nanocrystals and Diffuse Scattering

CLASSEThe ability to observe structural changes in biomolecules
while they function has been a goal of cellular biology formany decades. NMR is limited to tens of microseconds, theneed for large quantities of (often) isotopically-labeledmaterial, lengthy scan times, and difficulties of reaction
initiation in the NMR machine.
Time-resolved SAXS (Small Angle X-ray Scattering) & WAXS
(Wide-Angle X-ray Scattering) are valuable complements totime-resolved Laue crystallography, time-resolved laser
spectroscopy, and computational modeling - and increasingly
useful in studies of protein structure, function, and dynamics.
Time-resolved solution SAXS patterns are exquisitely
sensitive to protein volume changes and mass transport intoand out of the protein. Time-resolved WAXS fingerprints
Structural changes in myoglobin upon laser contain a wealth of structural information down to 2.5 Å,
flash photolysis of bound CO, as a proxy for and provide stringent constraints for models of
O2 binding, have been determined using Laue conformational states and structural transitions between them.
methods. The duration of the storage ring
pulse limited the time resolution to ~100 ps.
(from Cho et al., PNAS 2010 107,7281)

In practice, x-ray pulses are directed through a flow of
specimen solution to mitigate radiation damage. The minimum
time resolution achievable using x-rays from storage rings islimited by the x-ray pulse width to ~100 ps. ERLs improve thetime resolution of SAXS/WAXS to ~100 fs, orders ofmagnitude better than with present day storage rings.
33
KEK-IMSS 6 Dec 2011

Biomembrane Dynamics
M. Rheinstadter1, A. Fluerasu2, L. Lurio3, S. Mochrie4
Workshop 6: X-ray Correlation Spectroscopy using continuous beams

CLASSE

Increasing evidence suggests the presence
and importance of nanodomains, such as
rafts, In membrane function, yet suchdomains have not yet been directly
observed in a cell. Membrane properties
may also be strongly affected byinteractions and collective dynamics
between membrane-embedded proteins.
In both cases, the key interactions are likely
to occur at length scales of 1-100 nm, andover time scales of 10-6-10-2 seconds.

1Laboratory for Membrane and Protein Dynamics,

McMaster University and Canadian Neutron BeamCentre, NRC

XPCS, with the 2-3 orders of magnitude
increase in brilliance provided by an
ERL or USR, may reveal direct
signatures of such domains throughtheir fluctuations, which are beyond thereach of other techniques.
2NSLS-II, Brookhaven National Laboratory
3Department of Physics, Northern Illinois University
4Department of Physics, Yale University

34

KEK-IMSS 6 Dec 2011

Microscopic imaging of single chromosomes
Yoshinori Nishino, Hokkaido University
CLASSEWorkshop 1: Diffraction Microscopy, Holography and Ptychography using Coherent Beams

The chromosome is the package of DNA and proteins and its
structure is of utmost biological significance in understanding themechanism of faithful transmission of the genomic information fromone generation to the next. However, the structure of thechromosome is not well understood despite a long history of
research, because there has been no adequate microscopy tovisualize them. For example, conventional light microscopy does
not have enough resolution, and transmission electron
microscopy falls short of the penetration power to observe subcellular organelles intact.

Human Chromosome
Nishino, et al., PRL 102, 018101 (2009), from 38
images from -70 to +60 degrees, estimatedresolution of 120 nm, SPring-8 data.

X-ray diffraction microcopy (XDM) recently provided a newopportunity to visualize thick organelles, such as chromosomes, inthree dimensions with high image contrast. X-ray fluorescence
technique also provides a unique way to map a specific element in
sub-cellular organelles. For chromosomes, mapping phosphorus isespecially valuable as it provides how DNA backbones are internallyfolded.

By carefully controlling the radiation dose and employing cryopreservation, the high brilliance of an ERL or USR will
enable to effectively visualize organelles in 3D at 10 nm resolution.

35
KEK-IMSS 6 Dec 2011

Hard X-ray Nanoprobes
Jörg Maser & Stefan Vogt, Advanced Photon Source
Workshop 5: Materials Science with Coherent Nanobeams at the Edge of Feasibility

Structural phasetransition in VO2

diatoms

CLASSEThe study of complex materials on the nanoscale makes a multiprobe approach mandatory, in which multiple properties of such
multicomponent materials can be studied at the same time. The
CNM/APS nanoprobe combines a hard x-ray nanobeam of 40 – 50 nmwith high precision sample positioning. The microscope can run inscanning mode and in full-field mode using an additional condensor andx-ray imaging lens. Scanning images based on x-ray fluorescence andscattering contrast can be combined with nanoXRF mapping, and isused for strain mapping, studies of phase transition, and elemental
analysis. Moreover, nanobeam tomography yields 3D images inabsorption and phase contrast, with a 2D resolution of currently 30 nm.
Another nanoprobe community is forming in the biological, medical,
and environmental sciences. A second dedicated instrument wasdelivered recently. As an example, the microtomogram shows the 3D
elemental distribution in a sweet water diatom [de Jonge et al, PNAS,
107 (2010) 15676]. Diatoms are a major part of the phytoplankton andplay an important role in carbon sequestration in the oceans. Antherimportant application area are 3D element distributions in tissue
samples in medical studies, in particular for cancer research.

3 µm

element specificmicrotomogramof a diatom

An ERL or USR with its high coherent flux will enable ptychographic
Bragg coherent diffraction with curved wavefronts, which has thepotential to study structure and strain of both isolated and continuous
crystalline nanoscale regions in 3D, in complex matrices and in situ. The
approach was demonstrated by Hruszkewycz et al. [Optics Letters 36(2011) 2227]. At an ERL or USR such measurements could be
performed in a time-resolved fashion.
36
XDL2011 Science Case Summary,
September
1,2011
KEK-IMSS
6 Dec
2011

Structures of biological cells with < 10 nm resolution in 3D
Chae Un Kim, Cornell University
CLASSEWorkshop 1: Diffraction Microscopy, Holography and Ptychography using Coherent Beams
Visualization of sub-cellular components in 3D at high resolution isessential to understanding how cells function. However, the currently
existing microscopic techniques have limitations for this purpose. Optical
microscopy cannot provide high enough resolution (typically worse than 200nm) and electron microscopy is poorly suited for thick cellular samples,
requiring >1,000 sections.
X-ray diffraction microscopy (XDM) is a lensless microscopic technique anduses the high penetration power of X-rays to image biological cell (of a few
microns in size) at high resolution in 3D. XDM offers potential to image
whole cancer cells or the structure and connectivity of the subcellular organelles in 3D at 5-10 nm resolution.
The fundamental image resolution of XDM for biological samples is set byradiation damage. A variety of cryopreservation methods have beendeveloped, including ambient plunge-freezing and high-pressure
cryocooling techniques. The cryopreservation of hydrated samples replaces
water with either low-density amorphous (LDA) or high-density amorphous(HDA) ice. Both LDA and HDA ice exhibit density fluctuations, whose
structure and origins are presently poorly understood, which limit the use of
cryopreservation for XDM.
Probing local structures of HDA/LDA ice requires highly brilliant/coherent nano-focused X-ray beams. The X-ray
sources such as ERLs/USRs provide an ideal X-ray probe for this types of study. After better accounting for these density
fluctuations, we anticipate that the highly brilliant and coherent X-ray beams from ERLs/USRs will allow, for the
first time, study of cellular structures in 3D with 5 to 7 nm spatial resolution .
37
KEK-IMSS 6 Dec 2011

Micro x-ray beams and microfluidics to crystallize
and solve protein structure
Seth Fraden, Brandeis University
Workshop 2: Biomolecular Structure from Nanocrystals and Diffuse Scattering

CLASSE

Crystallization is the major bottleneck in the crystallographic
determination of biomolecular structure. Membrane proteins andmacromolecular complexes are particularly reticent to crystallize.
The key to optimizing crystallization is the separation of
nucleation and growth, and to obviate the need to grow large
crystals. To nucleate a crystal on a short enough time scale to bepractical requires a large supersaturation, which often leads to rapid
crystal growth and resulting in crystals which have defects and diffract
poorly. Microfluidic devices are being devised to temporarily bring theprotein solution into deep supersaturation where the nucleation rate ishigh and then, after a single crystal has nucleated, decrease thesupersaturation of the solution. This is done either by lowering theprotein or precipitant concentrations, or by raising temperature in orderto suppress further crystal nucleation and to establish conditions where
slow, defect free crystal growth occurs.
The result is a stream of microdrops, each containing a tiny single
crystal. These are conveyed sequentially at kHz rates into an intense
ERL/USR microbeam for a single diffraction pattern before radiation
damage destroys the crystal. Complete data sets are then obtained bymerging many diffraction patterns. Since the crystals are tiny and the
x-ray patterns are weak, x-ray source brilliance is essential toprovide sufficient flux density at the sample to obtain data sets inreasonable time.

XOp microfluidic chip optimizes crystal growth byvarying the degree of supersaturation versus time.
See www.elsie,brandeis.edu; Shim et al., JACS
127 (2007) 8825.
38
KEK-IMSS 6 Dec 2011

CLASSE

END

39
KEK-IMSS 6 Dec 2011