X-ray Free Electron Laser
Part-2 Photon Beamline andExperiments
XFEL Utilization Division, JASRI
Kensuke Tono

1

Contents
1. XFEL sciences
2. Photon beam properties
3. Photon beamline: Optics and diagnostics
4. Experimental stations
5. Experiments at SACLA

2

Contents
1. XFEL sciences
2. Photon beam properties
3. Photon beamline: Optics and diagnostics
4. Experimental stations
5. Experiments at SACLA3

XFEL properties and sciences• Short pulse (<10 fs)• High peak power (>60 GW)• Coherent
Ultrafast observation beyond the speed of atomic motion(Femtosecond snapshot)• Beyond static image
 Imaging functions (motion pictures of chemical
reaction, phase transition, etc.)• Beyond statistical image
 Imaging fluctuations, rare events
Ultrahigh intensity opens new regime of
X‐ray‐matter interactions• Beyond linear response4Femtosecond snapshot
Imaging of a live cell

Damage‐free protein crystallography

Suga, Shen et al., Nature (2015).
Kimura, Nishino et al., Nat. Comm. (2013).

Photosystem II (PSII)

Reaction center

Ultrafast dynamics in chemical reaction

Kim, Ihee, Adachi, et al., Nature (2015).
5Ultrahigh intensity application:
X‐ray nonlinear optics
50 nm focusing ⇒ ~1020 W/cm2
Amplification of x‐ray pulse using
Multiphoton process2‐pulse XFEL

Yoneda et al., Nature (2015)

Tamasaku et al., Nat. Photon (2014)

8 keV & 9 keV
Undulator

Cu foil（20 m）
Analyzer
Si (111)3500
Intensity (a.u.)

3000

K12500
2000
1500

K21000
500
07960

8000

80408080

Photon energy (eV)8120

Contents
1. XFEL sciences
2. Photon beam properties
3. Photon beamline: Optics and diagnostics
4. Experimental stations
5. Experiments at SACLA7

Properties of SASE XFEL beam
Low emittance & short pulse••••

Source size ~30 μm@10 keV
Divergence ~2 μrad@10 keV
Bandwidth ~5x10‐3Pulse duration <10 fs

Coherent
Transverse only
Multimode in longitudinalHigh intensity••

Pulse energy ~0.6 mJ @10 keV(~4x1011 photons)
Peak power >60 GW@10 keV

100intensity (a.u.)

••

120

80
60
40
200-2-1012

Relative photon energy (eV)

Shot‐by‐shot fluctuation
8Coherent (transverse only)Interference between scatteringwaves from two particles

Inoue (U. Tokyo) et al.,IUCrJ, in press (2015)

6 keV

Total degree of coherence: ~0.6~80% of the total power is in the dominant mode (TEM00)
9Multimode
Spectrum of single XFEL pulse consists of thousands of spikes
due to multi optical modes.
Si(111)Si(555)120

0x10100

intensity (a.u.)

120
Intensity (a.u.)

290 meV

3100
80
60

80
60
40

40
20

200

9.90

9.95

10.00

10.05

Photon energy (keV)

10.10-2-1

012

Relative photon energy (eV)Y. Inubushi et al., Phys. Rev. Lett. 109, 144801 (2012).

10Spectra
at different
pulse
durations
Evaluationof pulse
duration using
XFEL simulation
Inubushi et al., Phys. Rev. Lett.
109, 144801 (2012)(a) ΔE=110 meV(b)ΔE=290 meV(c) ΔE=600 meV(d) t=31 fs(e) t=8.9 fs(f) t=4.5 fs(FWHM)(FWHM)

MeasuredSpectraSimulated
spectra11

Shot‐by‐shot fluctuation
Intensity/position

Spectrum

Photon‐beam parameters and experimental data
should be collected in a shot‐by‐shot manner.
12

Contents
1. XFEL sciences
2. Photon beam properties
3. Photon beamline: Optics and diagnostics
4. Experimental stations
5. Experiments at SACLA

13

Design concept• Main optics & diagnostics are centralized inOptics Hutch‐> Transport & online diagnostics of a photon beam withlow emittance, short pulse, and high coherence.
‐> Fine electron‐beam tuning with X‐ray optics &diagnostics.

• Experimental stations provide only basic
infrastructure (e.g., optical laser, focusing system)‐> Enough space for various experimental instruments
14

SACLA Photon Beamline
BL3

BL1：SX
BL2: HX
BL3: HX

OH: Common optics& diagnostics

BL1BL2EH1: Beam diagnostics(Spectrum, timing)
EH2: Pump & Probe
w/ unfocused beam
EH3: 1-um focusing(Imaging, crystallography)
EH4: 1-um focusing(Nonlinear,Pump & Probe )Laser booth(CPA, OPA)SACLA-SPring-8
Experimental Facility
EH6: HEDS

EH5:
nanometerfocusing

High power laser

Common optics in optics hutch
Transport XFEL beam & filter out unnecessary lights• Double plane mirrors (2 sets): Low‐pass filter (Bandwidth of output
beam ~5x10‐3)• Double crystal monochromator (DCM, Si 111): Band‐pas filter (~1x10‐4)< 7.5 keV
< 15 keV

16

Damage/speckle free optical elements
XFEL features

Damage on a mirror material

Need toavoid…

Short pulse (<10 fs)⇒ DamageHigh peak power (>60 GW)
Coherent⇒ Wavefront
distortion

Typical Be window Speckle‐free Be window

Goto et al., Proc. of SPIE 6705 (2007)

Koyama et al., Opt. Exp. 21 (2013)

Ultraprecise mirror finished by
Elastic Emission Machining

Mimura et al., Rev. Sci. Instrum. 79, (2008)17

On‐line photon diagnostics:
Wavelength (photon‐energy) monitor
Photon energyCCDDiffracted beam
2θXFEL
Measurable range: 6 - 20 keV

Nano diamond film
7060502 (deg)

Wavelengths (λ) are calculated frompositions of Debye‐Scherrer rings onMPCCD.

40
30
Dia(111)Dia(220)
Dia(311)202dsinθ = nλ100
6810121416

photon energy (keV)181820Shot‐by‐shot measurement
photon energy

Trendphoton energy (keV)

10.0

Peak position
9.747±0.012 keV

9.9
9.8
9.7
9.6
9.5
050

100

150

200

shot number

shot number
19Arrival timing monitor
Intense X-ray irradiation induces opticaltransmittance change of a semiconductor(Spatial decoding technique)

Katayama –sanSato‐san (U. Tokyo)
T. Sato et al
APEX 8, 012702 (2015)

2D detector
SampleSi3N4,GIG,GaAs
Image of transmitted light(optical laser)

X-rays

Optical laser
OPA or CPA

two temperature model
Electron-electron scatteringof photoelectrons-> cascade hot-carrier
generation

Optical transmittancedecreases
S. M. Durbin, et al., X‐ray pump optical probe cross correlation study of GaAs Nature Photonics 6, 111 (2012)
M. Harmand, et al., Achieving few‐femtosecond time‐sorting at hard X‐ray free‐electron lasers Nature Photonics 7, 215 (2013)
N. Hartmann, et al., Sub‐femtosecond precision measurement of relative X‐ray arrival time for free electron lasers Nature Photonics 8, 706 (2014)
M. R. Bionta, et al., Spectral encoding method for measuring the relative arrival time between x‐ray/optical pulses Rev. Sci. Instrum. 85, 083116 (2014)

Contents
1. XFEL sciences
2. Photon beam properties
3. Photon beamline: Optics and diagnostics
4. Experimental stations
5. Experiments at SACLA21Single‐shot measurement is mandatory.
• Even a single pulse destroys a sample.

Neutze et al., Nature 406,752 (2000)• Pulse‐by‐pulse fluctuation of XFEL pulses.

Difficult to repeat measurementin the same condition.
22

Instrumentation for single‐shotmeasurement• High photon flux
 Focusing• Fast sample exchange Particle injectors
 Fixed targets with a fast scanning system• Fast & sensitive X‐ray detection
 High performance detector• Fast & reliable data acquisition (DAQ) High speed DAQ system with high performancecomputers & high speed network
 Large storage system

23

Focusing

Yumoto et al Nature Photon. 7, 43 (2013)

1‐um focusing mirrors

1.10.9First derivativeI / I00.70.540 µm
4 µm

0.30.1‐0.10102030

Wire position /a.u.

4050

Koyama et al, Opt. Exp. 21, 15382 (2013) 24

Particle injectors
Continuous beam

High‐viscosity sample

Droplets～0.5 μL/min～0.1 μL/min

He30 μm

Flow rate = ～ 0.4 mL/min
Proteins：～100 mg

Proteins：～0. 1 mg

Proteins：<0.1 mg

25

High‐performance detector
Kameshima , Hatsui et al., Rev.
Sci. Instrum. 85 (2014)• Multi‐port CCD (MPCCD)– High sensitivity– Low noise

Specification
Frame rate

• (single‐photon detection capability) Pixel size

– Fast (60 fps)
– Large area（□100 mm）

Octal Sensor Detector (100 x 100 mm)
2048 x 2048 pixels≥60 fps
50 μm

Noise

300e‐

Q.E.

~70 % @ 6 keV~20 % @ 12 keV

Dynamic range

14 bits

System noise< 0.2 ph.@ 6 keVFull well~ 3000 ph. @6keV~ 1500 ph. @12keV
26

Data acquisition (DAQ) system
Joti‐san, Kameshima‐san,Yamaga‐san, Hatsui‐san et al.

Data stream4 Gbps

Contents
1. XFEL sciences
2. Photon beam properties
3. Photon beamline: Optics and diagnostics
4. Experimental stations
5. Experiments at SACLA––––Coherent diffraction imaging (CDI)
Femtosecond protein crystallography
Time‐resolved X‐ray absorption spectroscopy (XAS)
Nonlinear X‐ray optics
28

Variety of research fields at SACLAFY 2013

FY 2012MI 0%
XQO 15%HEDS 11%
CHM&AMO
21%

BIO&CDI32%

PX 10%
MAT 11%MI 13%
XQO 12%HEDS 6%
CHM&AMO19%

FY 2014
BIO&CDI19%
PX 12%

MAT 19%MI 0% BIO&CDI14%
XQO 18%HEDS 6%
PX 14%MAT
CHM&AMO
21%
27%

BIO:

Imaging biology

AMO:

AMO science

CDI:

Coherent diffraction imaging

HEDS:

High energy density science

PX:

Protein crystallography

XQO:

X‐ray quantum optics

MAT:

Ultrafast materials scienceMI:

Methods and instrumentation

CHM:

Ultrafast chemistry~50 proposals accepted in a year (acceptance ratio ~50%)
29

XFEL as a probe, as a trigger• Observation in a “diffraction‐before‐destruction”
scheme.
– Coherent diffraction imaging (CDI)– Femtosecond protein crystallography (PX)

• Observation of ultrafast phenomena– Time‐resolved X‐ray spectroscopy• Light‐matter interaction under intense X‐rayirradiation: XFEL as a trigger of novel opticalphenomena– Nonlinear X‐ray optics, X‐ray amplification

30

“Diffraction before destruction” (1)CDI for single‐particle structure analysis
Differential scatteringcross section

Diffraction pattern

Structure factor

Electron density

Phase retrieval

SampleImages from Kimura et al., Nature Comm. 5,3052 (2013).

Fourier transform

Real-space image

Sample-image
reconstruction

31

Typical setup for CDIDetector 2

Detector 1

Sample loader
Sample chamber

Focusing optics

XFELFilterDetector 2

Detector 1
Kameshima et al., Rev. Sci. Instrum 85, 033110 (2014)

32

CDI of live cell
Kimura et al., Nature Communications 5, 3052 (2013).

33

CDI of nanomaterials
Metal nano‐cubes [Takahashi et al., Nano Lett. (2013)]
Resolution ~7 nm

3D structure of gold nanocrystals [R. Xu et al., Nat. Comm. (2014)]
Resolution ~5.5 nm

34

“Diffraction before destruction” (2)Femtosecond protein crystallography• Damage free– Room temperature measurement• Dynamics– Pump‐probe capability• Two major methods– For large, high‐quality crystals– For small crystals

35

Femtosecond crystallography
Hirata et al., Nature Methods 7, 735 (2014).

Damage‐free structure36Damage‐free structure of photosystem II
Structure of photosystem II

Possible mechanism for theoxygen evolving reaction.
WaterMnOH

CaO

oxygen evolving complex whereoxidation of water into dioxygen
occurs.

Suga, Shen et al., Nature (2015)37

Serial femtosecond crystallography (SFX)
Sample loading

Diffraction patternInjector

Micro crystals

2D detector &Data acquisition(DAQ) system

10 μm(room temp.)

Focusing

Data analysis
High performancecomputer

XFELStructure38

Single‐shot diffraction patterns of Lysozyme
Lysozyme（Average crystal size: ~5 μm）
Electron density map

Resolution <2Å

Statistics
Shot number: 70,000
Number of Images with diffraction spots : 21723 (Hit rate： 31%)
Indexable images: 13,912 (20%)
Measurement time: 1 hour (20 Hz)
39

Time‐resolved measurements forprobing ultrafast phenomena• Time‐resolved X‐ray absorption/emission
spectroscopy (XAS/XES)• Time‐resolved X‐ray diffraction/scattering• Time‐resolved photoelectron spectroscopy• Ultrafast probe for high energy density
sciences– Laser shock compression of materials– Ultrafast probe of plasma
40Time‐resolved XAS for ultrafast chemistry

Katayama et al,
APL 103, 131105
Obara et al, OE
22, 1105 (2014)

Differential spectrum

Temporal evolution

Time‐resolved wide‐angle X‐ray scattering(WAXS) for tracing ultrafast structural change

Photo-excited species andtimescales of structuralchanges.
Kim, Ihee, Adachi, et al., Nature (2015).
42

Simultaneous measurement of time‐resolved X‐rayemission spectroscopy (XES) and WAXSXESWAXS
Bimetallic donor–acceptor complex: Modelsystem for artificial photosynthesis.

43

Light‐matter interaction under intense
X‐ray irradiation• Nonlinear phenomena via interaction withintense XFEL– Double core‐hole generation– Two‐photon absorption– Saturable absorption– Amplification of x‐ray pulse

44Nonlinear phenomena via interaction with intense XFELIntense XFEL pulse interacts with atoms within a time scalecomparable to a core‐hole lifetime.
• Multi‐photons can be involved.
• Core‐holeatoms can contribute to optical phenomena.
E0L
X‐rayKLK

Lifetime: fs ~ asNonlinear phenomena associated with core‐hole atoms
・ Double core‐hole generation
・ Two‐photon absorption
・ Saturable absorption
・ Amplification of x‐ray pulseTo obtain enough XFEL intensity for nonlinear phenomena
XFEL intensity (irradiance)

EI
S 
Focal spot
~10‐10 cm2 (= 100 nm x 100 nm)

Pulse energy~10‐4 J(W/cm2)

Pulse duration~10‐14 s

Focusing XFEL down to < 100 nm, an intensity reaches 1020 W/cm2

High intensity applicationK. Tamasaku et al, PRL Vol.111 (2013)

Emission from double core hole atoms• 100 uJ/10 fs = 10 GW (after 1‐μm KB)• Focusing size: ~1x1 μm2

1 μm focusing• 10 GW/(1 μm)2~ 1018 W/cm2
Double core hole of Kr47

2‐stage focusing for
creating nanometer spot

Mimura et al,
Nature Comm., DOI: 10.1038/ncomms 4539 (2014)
Beam profile
Wire scan profile
Gaussian 45nm(FWHM)

Beam profile
Wire scan profile
Gaussian 55nm(FWHM)

1.0
Intensity (arb. unit)

Intensity (arb. unit)

1.01020 W/cm2@ 10 keVVertical

0.845nm(FWHM)

0.6
0.4

Horizontal

0.8
0.6
0.4

0.2

0.2

0.0

0.0-600-300
0300
Position (nm)600〜10 nm

55nm(FWHM)

Protein-600

-300
0300
Position (nm)60048

X‐ray nonlinear optics: two‐photon absorption
50 nm focusing ⇒ ~1020 W/cm2

Tamasaku et al., Nature Photon. (2014)

K‐shell core‐hole of Ge (absorption edge: 11. 1 keV)is created by absorption of two 5.6‐keV photons
E0
5.6 keV

L5.6 keVKLKSaturable absorption at Iron K‐edge
50 nm focusing

SpectrometerIron foilSample

XFEL

scan

2-stage focusing system

3000

30
 (eV)

A b s o rp tio n c o e ffic ie n t (c m -1 )4000

201000.0

2000

0.5
fexc

1.0

1000

07105 7110

19271307135

9.6x10 W/cm
192
7.9x10 W/cm
182
8.7x10 W/cm
182
1.9x10 W/cm
cold7115

7120 7125

Photon energy (eV)

Yoneda, Inubushi, et al.,Nat. Comm. (2014).

Amplification of x‐ray pulse using 2‐color XFEL
Prof. Yoneda(Univ. EC)

Pump pulse (9keV) creates core‐hole atoms.
Seed pulse (8keV) interacted with core‐hole atoms
is amplified by stimulated emission.
0.8

Pump
0.6

60
0.4

40
20SeedK1 (8.05keV)
K2 (8.03keV)

0
8.0

E

8.2

0.2

8.4
8.6
8.8
photon energy (keV)

Creation of core‐hole atom

09.0

transmission

intensity (a.u.)

80

0.0
9.2

Amplification bystimulated emission

L

PumpK

L

SeedK

Experimental setup
8 keV & 9 keV
Cu foil（20 m）

Undulator
2-stagefocusing system

2-color XFELMPCCDcamera

11 ID
8 ID

Electronbeam

Analyzercrystal
Si (111)2‐color
XFEL

9.05 keV: K=1.92
8.05 keV: K=2.1

T. Hara, et al, Nature Comm. 2013

Amplification of x‐ray pulses
Intensity：5x1019 W/cm2

K2
K1

Photon energy

Photon energy

Intensity：1x1018 W/cm2

K2
K1

Spectrum of amplified x‐ray pulse
Single‐shot spectrum
3500
K1

Intensity (a.u.)

3000
2500

K2

2000
1500
1000
500
07960

8000

8040

8080

8120

Photon energy (eV)

We achieved amplification of x‐ray pulse.
・ Creation of population inversion by intense XFEL pulses
・ Confirmation that XFEL pulses are applicable as seed pulses

Summary• Novel properties and sciences of XFEL– Ultra‐brilliant, ultra‐short, and coherent X‐ray pulses– Beyond static, statistical pictures• Beamline for XFEL
– Damage‐free & speckle‐free optics– Single‐shot, nondestructive diagnostics• Experimental instrumentation for single‐shot measurement– Focusing optics, sample injectors, detectors, DAQ system,
femtosecond laser• Experiments at SACLA– Femtosecond snapshot of sample; “diffraction before destruction”– Ultrafast science by pump‐probe measurement– X‐ray‐matter interaction under ultra‐high intensity
55

Outlook• Upgrade of SACLA– Double‐pulse operation– Multi‐beamline operation (BL1, BL2, BL3)
– Self seeding (under development)• New instruments– Experimental platforms for time‐resolved measurement• SFX• X‐ray spectroscopy– Ultimate focusing– High power lasers (500 WT x 2)
– Detector upgrade• Vacuum‐compatible MPCCD module• MPCCD phase III for higher sensitivity• SOPHIAS for wider dynamic range, small pixel
56