Toward Fourier-limited X-ray Science

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1 XDL2011 RPCC, Cornell Univ. June 20-21, 2011 GRC X-ray Science 2009 Colby College August 2-7, 2009 Toward Fourier-limited X-ray Science Photon Factory, KEK & PREST, JST Shin-ichi Adachi

2 outline Time-domain X-ray science with Storage Ring (Photon Factory Advanced ring, KEK) Current status of Energy Recovery Linac (ERL) project at KEK MeV ERL test facility (under construction) 3.5GeV ERL + XFEL Oscillator (not approved) Towards Fourier-limited X-ray Science with XFEL-O and seeded XFEL Inelastic X-ray scattering Nonlinear X-ray Optics Two-photon correlation spectroscopy Transient grating Summary

3 outline Time-domain X-ray science with Storage Ring (Photon Factory Advanced ring, KEK) Current status of Energy Recovery Linac (ERL) project at KEK MeV ERL test facility (under construction) 3.5GeV ERL + XFEL Oscillator (not approved) Towards Fourier-limited X-ray Science with XFEL-O and seeded XFEL Inelastic X-ray scattering Nonlinear X-ray Optics Two-photon correlation spectroscopy Transient grating Summary

4 TR x-ray applications at KEK Picosecond photoresponse of perovskite manganite (NSMO) thin film (~ 50ps ~ 2ns) Photo-induced spin-crossover transition of metal complex in solution (TR-XAFS: ~700ps) Photochemical reaction in liquid (TR-liquidography: ~100ps~1s) Ligand migration dynamics in protein crystal (~800 min) Laser shock-induced lattice deformation of CdS single crystal (TR single-shot Laue diffraction: ~1ns~10ns)

5 PF AR (6.5GeV) Full Time Single Bunch Operation ~200days/year multilayer mirror Si(111) monochromator undulator beamline NW14A at PF-AR femtosecond laser system nanosecond laser system Jülich x ray chopper

6 #1 TR Diffraction Picosecond photoresponse of perovskite manganite (NSMO) thin film 1 khz rep rate with mono X ray (E/E ~ 0.01%) ~10 9 photons/sec

7 Phase Transition in Manganite Thin Film Nd 0.5 Sr 0.5 MnO 3 /SrTiO 3 (011) (NSMO/STO(011)) (Nd,Sr) Ichikawa et al. Nature Materials, 10, (2011) MnO 6 thickness: 80 nm e g Mn 3+ : (3d) 4 x 2 y 2 3z 2 r 2 Nakamura et al. APL (2005) CE-type Antiferromagnetic insulator (CE-AFI) Ferrometal (FM) t 2g

8 Optical pump-probe results Collaboration with K. Miyano Group (Univ. of Tokyo) TR-Reflectivity (100K) Kerr Rotation Ichikawa et al. Nature Materials, 10, (2011) Miyasaka et al. PRB (2006)

9 Temperature dependence of X-ray Diffraction CCD Image T = 180 K (004) H T = 140 K T = 100 K (004) L (040) L Intensity (arb.) (040) L 6.5 (004) H 6.6 Q (Å -1 ) Nd 0.5 Sr 0.5 MnO 3 /SrTiO 3 (011) T = 180 K T = 140 K T = 100 K (004) L Heating Lattice parameter (Å) Intensity (arb.) b c a b HT, c HT (1/4 9/4 0) (1/2 3/2 2) Temperature (K) 180 CE-AFI (charge/orbital order) FM cluster (charge/orbital disorder)

10 Layout of the laser-pump X-ray-probe experiment Pump Laser 800 nm (1.55 ev) FWHM: 150 fs Ti:Sapphire PF-AR Detector (CCD, Scintillation counter) XPS X-ray Energy: 15 kev FWHM: 100 ps CCD Sample NSMO/STO(011) thin film Film thickness: 80 nm Laser X-ray Sample

11 Time dependence of (004) reflection Nd 0.5 Sr 0.5 MnO 3 /SrTiO 3 (011) Difference Image black white (004) L (040) L T = 100 K (040) L (004) L (004) L (040) L T = 100 K Pump: 0.8mJ/cm 2

12 Time dependence of the (004) and (1/4 9/4 0) reflections Nd 0.5 Sr 0.5 MnO 3 /SrTiO 3 (011) T = 100 K Pump: 0.8mJ/cm 2 Lattice Expansion (Å) Relative Intensity c-axis b-axis (1/4 9/4 0) Delay Time (ps) c-axis b-axis (1/4 9/4 0) Delay Time (ps)

13 Photo-induced hidden state? Difference Intensity (arb.) Temperature Dependence (Without laser irradiation) 120 K 115 K 110 K 106 K 102 K 180 K (0.05) Pump Power Dependence T = 100 K (Delay-time: +150 ps) 0.8 mj/cm mj/cm mj/cm mj/cm 2 Initial state FM cluster CE-AFI Q (Å -1 ) Q (Å -1 ) 6.7 Thermal-excitation Photo-excitation Photo-excited state Ichikawa et al. Transient photoinduced hidden phase in a manganite Nature Materials, 10, (2011)

14 #2. TR XAFS Photo-induced spin-crossover transition of metal complex in solution 1 khz rep rate with mono X ray (E/E ~ 0.01%) 10 9 photons/sec

15 Nozawa et al. J. Am. Chem. Soc., 132, (2010). photo-induced spin-state transition by TR-XAFS Fe 2+ (phen) 3 Shunsuke Nozawa (KEK) Tokushi Sato (KEK) Open Jet system Laser pulses 945 Hz Fluorescence X-ray X-ray 794 khz (Energy-scanned )

16 picosecond time-resolved spin-crossover transition of Fe II (phen) 3 LS state S=0, 1 A 1 HS state S=2, 5 T 2 e g Fe 2+ (phen) 3 3d 6 10Dq 1 MLCT t 2g Energy 400nm MLCT,LF FeN 6 cluster 5 T 2 1 A 1 (LS) ~700ps (HS) Fe N bond length R LS < Fe N R HS Fe N Fe N bond length

17 TR-XAFS: Experimental Setup

18 TR-Near Edge Structure Fe K-edge XAFS Fe(phen) 3 Aqueous Solution C D Time Course Feature B Intensity (arb. units) A B difference x 15 Intensity (arb. units) FWHM 142 ps X-ray = 60 ps I = I 0 exp[-(t/)] = ps Low Spin Transient difference at +50ps Time Course Feature D Photon Energy (ev) Delay (ps)

19 TR-XANES features in pre-edge region Fe(phen) 3 : Low Spin Fe(2-CH 3 phen) 3 : High Spin HS-LS Transient difference (+50ps) e g LS state S=0, 1 A 1 1 peak HS state S=2, 5 T 2 2 peaks Intensity (arb. units) Fe K-pre-edge difference x t 2g 7112 e g 7114 Photon Energy (ev) d 6 t 2g Intensity (arb. units) Dq Delay (ps) Time Course e g = 691 ps

20 excited state EXAFS Intensity (arb. units) Fe K-edge EXAFS LS Transient difference (+50ps) difference Fourier Transform LS transient HS (+50ps) Photon Energy (ev) Distance R (A) 3 4 EXAFS analysis summary Spectrum R Fe-N () 2 ( 2 ) LS 1.98(1) 0.001(1) Photo-excited HS 2.15(2) 0.011(3)

21 Low Spin State photoinduced structural change: a molecular movie! 1.98 Photoexcited High Spin State 2.15 Energy 1 MLCT 400nm MLCT,L F 1 A 1 (LS) ~700ps Fe N bond length 5 T 2 (HS) Nozawa et al. J. Am. Chem. Soc., 132, (2010).

22 TR-XAFS - summary Low Spin State Photo-Excited High Spin State 1.98Å h (400nm) 700ps 2.15Å TR XAFS provides spin, electronic and structural information of photo induced states, which enables to produce molecular movies.

23 outline Time-domain X-ray science with Storage Ring (Photon Factory Advanced ring, KEK) Current status of Energy Recovery Linac (ERL) project at KEK MeV ERL test facility (under construction) 3.5GeV ERL + XFEL Oscillator (not approved) Towards Fourier-limited X-ray Science with XFEL-O and seeded XFEL Inelastic X-ray scattering Nonlinear X-ray Optics Two-photon correlation spectroscopy Transient grating Summary

24 Evolution of the synchrotron sources source Case1: 3 rd gen. synchrotron sources Case2: ERL & SASE-XFEL (Diffraction limit) Case3: XFELO & seeded XFEL (Fourier limit)

25 Diffraction Limit ERL & SASE-XFEL x x' 4

26 Fourier Limit XFELO & seeded XFEL t 4 h

27 Fourier limited X ray E ev mev ev XFELO Seeded XFEL? kev ns ps fs as t

28 KEK Energy Recovery Linac (ERL) project Linac based light source: 1) Diffraction-limited beam ~15pmrad ~λ/4π 2) Short pulse capability 0.1~1 pico-second 3) High repetition rate 1.3 GHz

29 35-245MeV ERL test facility (Compact ERL) - Plan and Status -

30 Compact ERL for developing and demonstrating ERL technologies Parameters of the Compact ERL Parameters Beam energy Injection energy Average current Acc. gradient (main linac) Normalized emittance Bunch length (rms) RF frequency MeV 5 MeV ma 15 MV/m mm mrad 1-3 ps (usual) ~ 100 fs (with B.C.) 1.3 GHz ERL Development Hall 100 m

31 Recent View in the ERL Development Hall (EDH) Clean Room for SCC Assembly Liquid Helium Refrigerator 32

32 3.5GeV ERL (1 st phase) + XFELO (2 nd phase)

33 3.5GeV ERL Plan at KEK Parameters of the ERL KEKB Beam energy Parameter 3.5 GeV 3.5 GeV ERL + XFELO Average current ma Normalized emittance mm mrad Energy spread (rms) (0.5-2) 10-4 PF-AR PF Bunch length (rms) RF frequency 1-3 ps (usual mode) ~ 100 fs (bunch compression) 1.3 GHz Parameters of the light sources ERL Development Hall (Compact ERL) Spectral range Average brilliance from insertion devices Average flux Parameter 30 ev - 30 kev ph/s/mm 2 /mrad 2 /0.1%bw > phs/s/0.1%bw 400 m Number of ID s

34 ERL undulator spectra (with 15pmrad ~ 1.5nmrad natural emittance) E=3.5GeV I=100mA x=y=5m K=1.0 E /E=4e-5 L=5m u=16mm

35 1 st harmonic of the undulator ev) (with 15pmrad ~ 1.5nmrad natural emittance) E=3.5GeV I=100mA x=y=5m K=1.0 E /E=4e-5 L=5m u=16mm Undulator radiation I ( ) sin N N 2

36 1 st harmonic of the undulator (linear scale) E/E = 12 ev / 4024 ev = E=3.5GeV I=100mA x=y=5m K=1.0 E /E=4e-5 L=5m u=16mm /=1/N N = 5000/16 = 313 1/N = 16/5000 =

37 Courtesy of K. J. Kim

38 Low emittance and high rep rate of ERL matches the specs of XFEL Oscillator (XFELO) Electron beam: Energy 7 GeV Bunch charge ~ pc Bunch length (rms) ps Normalized rms emittance < mm mr Energy spread (rms) ~ 2x10 4 Constant bunch rep ~1 MHz Undulator: L u = m, u =2.0 cm, K= Optical cavity: 2 or 4 diamond crystals and focusing mirrors Total round trip reflectivity > % XFELO output: K.-J. Kim et al. PRL (2008) 100, kev 25 kev Bandwidth: ~ 1 x 10 7, pulse length (rms) = fs # photons/pulse ~ 1x10 9

39 Energy Recovery Linac (ERL) and XFEL Oscillator 7 GeV XFEL O 3.5 GeV main SC linac

40

41 Seeded XFEL & XFELO Seeded XFEL =10-6 cf. K.-J. Kim et al., PRL 100, (2008).

42 outline Time-domain X-ray science with Storage Ring (Photon Factory Advanced ring, KEK) Current status of Energy Recovery Linac (ERL) project at KEK MeV ERL test facility (under construction) 3.5GeV ERL + XFEL Oscillator (not approved) Towards Fourier-limited X-ray Science with XFEL-O and seeded XFEL Inelastic X-ray scattering Nonlinear X-ray Optics Two-photon correlation spectroscopy Transient grating Summary

43 Fourier limited X ray E ev mev ev XFELO Seeded XFEL? kev ns ps fs as t

44 1. inelastic X ray scattering Current High Resolution APS, ESRF, SPring photons/sec, E~1meV XFELO X-ray beam characteristics 1x10 9 1MHz 1x10 15 photons/sec ~ 10-7 Ideal for IXS, NRS, HXPES, etc APS XFELO Workshop 2010 Presentation by Clement Burns (Western Michigan Univ.)

45 2. Nonlinear X ray Optics Quantitative and systematic studies will require Fourier-limited X-rays Sum- & difference-frequency mixing applications Parametric down-conversion X (pump) X (signal) + EUV or SX (idler)

46 3. two photon correlation spectroscopy1 in radio wave domain t frequency MHz (10 6 Hz) GHz (10 9 Hz) THz (10 12 Hz) PHz (10 15 Hz) EHz (10 18 Hz) wavelength 0.3km (10 3 m) 0.3m (10 0 m) 0.3mm (10-3 m) 0.3m (10-6 m) 0.3nm (10-9 m) Radio wave domain Multi-dimensional NMR Correlation of nuclear magnetic spin

47 two photon correlation spectroscopy 2 in IR domain t frequency MHz (10 6 Hz) GHz (10 9 Hz) THz (10 12 Hz) PHz (10 15 Hz) EHz (10 18 Hz) wavelength 0.3km (10 3 m) 0.3m (10 0 m) 0.3mm (10-3 m) 0.3m (10-6 m) 0.3nm (10-9 m) IR region Multi-dimensional IR spectroscopy (photon echo) Correlation of vibrational modes

48 two photon correlation spectroscopy 3 in X ray domain t frequency MHz (10 6 Hz) GHz (10 9 Hz) THz (10 12 Hz) PHz (10 15 Hz) EHz (10 18 Hz) wavelength 0.3km (10 3 m) 0.3m (10 0 m) 0.3mm (10-3 m) 0.3m (10-6 m) 0.3nm (10-9 m) X-ray region Multi-dimensional X-ray spectroscopy Correlation of electronic states, Wave packet motion?

49 4. Transient grating Transient X ray standing wave without perfect crystal Transient grating with fully coherent X-ray X-ray standing wave Proposed by Keith Nelson Standing wave

50 Summary SC Linac based light source enables electron beam with high rep rate and low emittance suitable for Fourier limited X ray sources. Fourier limited X ray may open new X ray applications in inelastic X ray scattering, nonlinear X ray optics, two photon correlation spectroscopy and transient grating.

51 Beam Line NW14A, KEK Shunsuke Nozawa (KEK) Tokushi Sato (KEK) Manabu Hoshino (TITECH) Ayana Tomita (KEK) Matthieu Chollet ( APS) Laurent Guérin ( Univ. Rennes 1) Hirohiko Ichikawa (JST) Shin-ya Koshihara (TITECH)

52 Recovery from the earthquake Earthquake epicenter Fukushima Daiichi KEK Damages at KEK March 11, 2011 Photon Factory now operating! Top-up mode June 20, 2011

53 Thank you for your attention

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