Pump/Probe Experiments

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1 Cheiron School 2008 Pump/Probe Experiments T. Gejo (University of Hyogo) Today s Topics Univ. of Hyogo? Where is it? General aspects of pump/probe experiments Laser/Synchrotron pump/probe experiments FEL/Laser pump probe experiments Storage-Ring-FEL/SR pump probe experiments 1

2 Today s Topics Univ. of Hyogo? Where is it? General aspects of pump/probe experiments Laser/Synchrotron pump/probe experiments FEL/Laser pump/probe experiments Storage-Ring-FEL/SR pump/probe experiments 2

3 What is pump/probe experiment? Laser(probe) exited state Pulse laser (Nano second, or femto second Laser) Laser(pump) ΔT ground state Time dependent measurements Spectroscopy Quantum Information Basic scheme of pump/probe experiments Fluorescence Ions Electrons probe pump Wavelength ΔT ΔT 3

4 Other spectroscopic techniques of pump/probe experiments Fluorescence Threshold Ions Electrons pump probe probe ΔT pump ΔT Wavelength of probe Depletion technique Stimulated Emission Pumping technique Wavelength of pump Example pf pump/probe experiment 4

5 One of the examples (Angular distributions of photoelectrons) "Non-adiabatic dynamics effects in Chemistry revealed by time-resolved charged particle imaging" Toshinori Suzuki and Benjamin J. Whitaker, Int. Rev. Phys. Chem.20, 303 (2001). Today s Topics Univ. of Hyogo? Where is it? General aspects of pump/probe experiments Laser/Synchrotron pump/probe experiments FEL/Laser pump/probe experiments Storage-Ring-FEL/SR pump/probe experiments 5

6 Laser/Synchrotron pump/probe experiments SR(pump) exited state Laser(probe) Laser(probe) SR(pump) exited state ΔT ground state ΔT ground state Time dependent measurements : photoelectron spectra, X-ray diffraction Spectroscopy of highly excited state One big difficulty of pump/probe experiments with Laser/SR Laser SR SR Laser Laser Ionization potential exited state Signals due to SR only gives high Back ground noise ground state When you measure of photoelectron spectra. Other problems X-ray penetrates deeper. Repetition frequency of the pump-probe experiment is limited by sample. 6

7 Examples 1 IR and Laser spectroscopy at UVSOR Excited state Relaxation IR absorption Two photon excitation Ground state J. Azuma, M. Kamada, M. Itoh et al. (UVSOR) PbBr 2, PbCl 2 7

8 Experimental set up Storage Ring Ti:sapphire hn=3.0ev 1 khz 150 fs BL-6A1 BL-6A2 Bruker sample Laser DO.D. Results PbBr 2 T=13K PbBr 2 PbCl 2 Laser ON -) Laser OFF PbCl 2 T=13K DO.D. DO.D Wavenumber (cm -1 ) J. Azuma, M. Kamada, M. Itoh et al. 8

9 Examples 2 T. Tsujibayashi, et al. PRL (2005) 9

10 BaF 2 T. Tsujibayashi, et al. PRL (2005) AF luminescence detected by dual MCA system Laser Timing laseron (a)laser (3.1 ev) +SR (18.4 ev) Accumulated for 2700 sec. Time evolution of AF luminescence with laser (laser ON) and without laser (laser OFF). Counts LaserOFF (b)sr (18.4 ev) Accumulated for 2700 sec Time (ns) 10

11 BaF 2 T. Tsujibayashi, et al. PRL (2005) Examples 3 11

12 Time-resolved X-ray Scattering Observe the change of diffraction pattern!! X-ray (probe) pump ΔT ΔT Time (ns) Time (ns) X-ray laser laser X-ray DVD disks S. Kimura, Y. Tanaka et al. (JASRI, RIKEN) 12

13 2/21-filling+18 bunches ns S. Kimura, Y. Tanaka et al. (JASRI, RIKEN) 13

14 Today s Topics Univ. of Hyogo? Where is it? General aspects of pump/probe experiments Laser/Synchrotron pump/probe experiments FEL/Laser pump/probe experiments Storage-Ring-FEL/SR pump/probe experiments Examples (Germany) 14

15 Experiments at FLASH FEL energy: X-rays 20fs, ~20 µj/pulse. Optical Laser: 800 nm or 400 nm, 130fs, 10µJ/pulse. C. Gahl, A. Azima, M. Beye, M.Deppe, K. Döbrich, F. Hennies, A. Melnikov, M. Nagasono, M. Wolf, W. Wurth, A. Föhlisch Nature Photonics (2008). How to adjust timing between Laser and FEL? 15

16 Synchronization of FEL and Laser at Spring-8 FEL RF 5712 MHz, 238 MHz, 79.3 MHz Mode Locked Ti:Sapphire Laser with 79.3MHz + Amplifier (Chirp plus Amplifier, CPA) = 1 khz Today s Topic Univ. of Hyogo? Where is it? General aspects of pump/probe experiments Laser/Synchrotron pump/probe experiments FEL/Laser pump/probe experiments Storage-Ring-FEL/SR pump/probe experiments 16

17 UVSOR Storage ring FEL at UVSOR Optical cavity length = 13.3 m = ( Ring circumference)/4 Electron Bunch Electron Bunch 17

18 Laser + SR Advantage :High energy resolution :Time-dependent measurement SRFEL + SR Advantage :No jitter (Natural synchronization) :Higher photon flux (~1W) :Lasing is is possible with wide region of of wavelength UVSOR-II-FEL の短波長化 nm Wavelength (nm) 18

19 Introduction of pump/probe experiments FEL SRFEL at at UVSOR Wavelength Intensity Frequency nm nm MAX 1.2W (( ~100nJ) 10MHz Experiment Sample Pump light Probe light Xe Xe Undulator light + LIF filter VUV SR FEL Energy Diagram of Xe 13.4 ev Xe + 5p 5 ( 2 p 1/2 ) 12.6 ev 12.1 ev 10.4 ev FEL 5p 5 ( 2 p 1/2 )4f'[5/2] Xe + 5p 5 ( 2 p 3/2 ) 5p 5 ( 2 p 3/2 )5d[3/2] 1 1 decay: t=600 ps SR Xe 5p 6 ( 1 S 0 ) Energy Diagram of Xe 19

20 Imaging technique Beam Nozzle MCP+PSD Extractor Repeller SR light FEL Transport FEL Mirror Optical Klystron FEL Mirror beam bunch FEL beam bunch Undulator Mirror f = m 5 m 10 m 20

21 Future Plan FEL Mirror FEL Mirror 1850 mm FEL beam bunch A 1250 mm 7560 START POINT Blue Poles( H: 1650 mm) C END POINT beam bunch 19 deg. B D B) A) SR Q1 2000F100 E 500 DELAY: 60 ~ 660 New tabel( H: 1650 mm) A) Hight : B) Hight : BL7B Optics 5 Laser size s (mm) laser waist f = 10 m f = 2m Length from backward mirror (m) 21

22 Timing Undulator light LiF Lens In vacuum Xe gas FEL 50 FEL Sampling Optical Oscillosope Movable optical delay stage Intensity (a. u.) 30 SR Time (nsec) 22

23 23

24 Synchronization of FEL and SR pulses 300x Undulator Intensity (count/sec) Intensity FEL 2s = ns 2s = ns timedelay (ns) time (ns) 4 5 Ion yield spectrum Intensity 120x q = ± s b = ± 0 s a = ± 144 g = ± x0 = ± x10 3 Wavenumber (1/cm) 24

25 Ion yield spectrum with changing wavelength of SR Intensity (counts/sec) Torr 2000u-2000u Intensity (counts/sec) Torr 500u-500u Wavelength (nm) Wavelength (nm) Energy Diagram of Xe Xe + 5p 5 ( 2 P 1/2 ) FEL 5p 5 ( 2 P 1/2 )4f {5/2} Xe + 5p 5 ( 2 P 3/2 ) 5p 5 ( 2 P 3/2 )5d{3/2} SR FEL SR SR FEL 25

26 Polarization effect Intensity (counts/sec) 50x Vertical Horizontal Circular Normal FEL wavelength (nm) Experiment with Q-switching FEL 0 ms 50 ms 100 ms 0 ns FEL 1.9 ns Event Gate 26

27 Q-switching FEL 18x Intensity (counts/sec) FEL wavelength (nm) 300x Intensity (counts/sec) FEL wavelength (nm) Today s Topics Univ. of Hyogo? Where is it? General aspects of pump/probe experiments Laser/Synchrotron pump/probe experiments Laser/FEL pump/probe experiments Storage-Ring-FEL/SR pump/probe experiments 27

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