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C. Laulhé, S. Ravy, P. Fertey, E. Elkaïm, F. Legrand

Studies of ultrafast structural changes at SOLEIL synchrotron: sub-ns and sub-ps pump-probe diffraction on CRISTAL beamline. C. Laulhé, S. Ravy, P. Fertey, E. Elkaïm, F. Legrand. (CRISTAL beamline - SOLEIL synchrotron). Ph. Hollander, S. Hustache, J.-P. Ricaud, P. Féret, T. Moreno.

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C. Laulhé, S. Ravy, P. Fertey, E. Elkaïm, F. Legrand

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  1. Studies of ultrafast structural changes at SOLEIL synchrotron: sub-ns and sub-ps pump-probe diffraction on CRISTAL beamline C. Laulhé, S. Ravy, P. Fertey, E. Elkaïm, F. Legrand (CRISTAL beamline - SOLEIL synchrotron) Ph. Hollander, S. Hustache, J.-P. Ricaud, P. Féret, T. Moreno (SOLEIL synchrotron) M.-L. Boillot (Institut de Chimie Moléculaire et Matériaux d’Orsay) E. Collet, M. Lorenc, M. Buron-Le Cointe, H. Cailleau (Institute of Physics - Rennes) ANR ULTiMATE – « ULTrafast co-operative and coherent photo-switching of molecular MATErials »

  2. Outline Studies of ultrafast structural changes at SOLEIL synchrotron: sub-ns and sub-ps pump-probe diffraction on CRISTAL beamline • Pump-probe diffraction: how ? • Pump-probe diffraction: motivations • Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 • Summary

  3. Outline Studies of ultrafast structural changes at SOLEIL synchrotron: sub-ns and sub-ps pump-probe diffraction on CRISTAL beamline • Pump-probe diffraction: how ? • Pump-probe diffraction: motivations • Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 • Summary

  4. Pump-probe diffraction • Following photoinduced structural changes as a function of time Δt RX 80 fs // 70 ps Laser h = 1.55 eV Undulator 25 fs • Toward ultrashort X-ray pulses at SOLEIL synchrotron… • → Natural temporal width of a synchrotron X-ray pulse: 70 ps FWHM • → « low- » mode: 10 ps FWHM (preliminary tests in Dec 2011) • → « Slicing » mode: 80 fs FWHM (2014) Making a movie of structural evolutions on the timescales of atomic vibration E ~ 10 meV ↔ Tosc ~ 400 fs

  5. CRISTAL: future installation for pump-probe experiments Undulator 6-circle 4-circle 36.00 m 31.25 m 0 m

  6. CRISTAL: future installation for pump-probe experiments • Ti:Sa oscillator + regenerative Ti:Sa amplifier •  = 800 nm, 25 fs FWHM • 500 µJ/pulse @ 10 kHz, 6 mJ/pulse @ 1 kHz ~ 1 ms (~ 1 kHz) Undulator 6-circle 4-circle 42.13 m 36.00 m 31.25 m 0 m

  7. 2.5 2.0 1.5 1.5 1.0 0.5 0.0 0 100 50 150 200 250 CRISTAL: future installation for pump-probe experiments • Ti:Sa oscillator + regenerative Ti:Sa amplifier •  = 800 nm, 25 fs FWHM • 500 µJ/pulse @ 10 kHz, 6 mJ/pulse @ 1 kHz ~ 1 ms (~ 1 kHz) 90 ns Delay Undulator 6-circle 4-circle 42.13 m 36.00 m 31.25 m 0 m x 106 XPAD detector Total intensity [a.u.] • Photon counting enabled on level high of a logic gate • Up to 847 kHz frequency Delay [ns]

  8. Outline Studies of ultrafast structural changes at SOLEIL synchrotron: sub-ns and sub-ps pump-probe diffraction on CRISTAL beamline • Pump-probe diffraction: how ? • Pump-probe diffraction: motivations • Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 • Summary

  9. Laser-induced phenomena in condensed matter • t = 0 : laser driven electronic transition → Out-of-equilibrium states → Decoupled degrees of freedom  = 800 nm ↔ E = 1.55 eV t : few fs

  10. 10 100 100 10 100 10 10 fs ps ns µs Diffracted intensity (a.u.) -0.5 0.0 0.5 1.0 1.5 Time (ps) Laser-induced phenomena in condensed matter • t = 0 : laser driven electronic transition → Out-of-equilibrium states → Decoupled degrees of freedom  = 800 nm ↔ E = 1.55 eV t : few fs Coherent phonons t < few ps : coherent phonons P. Beaud et al., PRL (2009) (5 3/2 2) La0.42Ca0.58MnO3 Sudden shift of the equilibrium coordinates of the ions: Displacive excitation

  11. 10 100 100 10 100 10 10 fs ps ns µs Diffracted intensity (a.u.) -0.5 0.0 0.5 1.0 1.5 Time (ps) Laser-induced phenomena in condensed matter • t = 0 : laser driven electronic transition → Out-of-equilibrium states → Decoupled degrees of freedom  = 800 nm ↔ E = 1.55 eV t : few fs Photoinduced ph. tr. Coherent phonons t < few ps : coherent phonons t < few 100 ps : ultrafast phase transitions P. Beaud et al., PRL (2009) VO2 T ˃ Tc T ˂ Tc Temperature (5 3/2 2) t0 t1 t2 Laser excitation La0.42Ca0.58MnO3 t0 Sudden shift of the equilibrium coordinates of the ions: Displacive excitation t2 P. Baum et al., Science (2007) t1

  12. 10 100 100 10 100 10 10 fs ps ns µs Diffracted intensity (a.u.) -0.5 0.0 0.5 1.0 1.5 Time (ps) Laser-induced phenomena in condensed matter • t = 0 : laser driven electronic transition → Out-of-equilibrium states → Decoupled degrees of freedom  = 800 nm ↔ E = 1.55 eV t : few fs Photoinduced ph. tr. Coherent phonons t in range [10 fs - 100 ps]: lattice dynamics driven by interactions with electronic degrees of freedom t < few ps : coherent phonons t < few 100 ps : ultrafast phase transitions P. Beaud et al., PRL (2009) VO2 T ˃ Tc T ˂ Tc Temperature (5 3/2 2) t0 t1 t2 Laser excitation La0.42Ca0.58MnO3 t0 Sudden shift of the equilibrium coordinates of the ions: Displacive excitation t2 P. Baum et al., Science (2007) t1

  13. 10 100 100 10 100 10 10 fs ps ns µs Laser-induced phenomena in condensed matter • t = 0 : laser driven electronic transition → Out-of-equilibrium states → Decoupled degrees of freedom  = 800 nm ↔ E = 1.55 eV t : few fs Photoinduced ph. tr. Strain waves Coherent phonons Heat diff. t ~ 1 - 100 ns : propagation of deformation waves t ~ 1 - 10 µs : laser-induced heat diffusion • Phonon creation: local increase of temperature • Heat diffusion: homogeneisation of temperature • Stressed regions: propagation of a strain wave compressive strain

  14. 10 100 100 10 100 10 10 fs ps ns µs Laser-induced phenomena in condensed matter • t = 0 : laser driven electronic transition → Out-of-equilibrium states → Decoupled degrees of freedom  = 800 nm ↔ E = 1.55 eV t : few fs Photoinduced ph. tr. Strain waves Coherent phonons Heat diff. t in range [100 ps - 10 µs]: Laser induced strain waves and heat diffusion - control of the electronic properties ?? t ~ 1 - 100 ns : propagation of deformation waves t ~ 1 - 10 µs : laser-induced heat diffusion • Phonon creation: local increase of temperature • Heat diffusion: homogeneisation of temperature • Stressed regions: propagation of a strain wave compressive strain

  15. Outline Studies of ultrafast structural changes at SOLEIL synchrotron: sub-ns and sub-ps pump-probe diffraction on CRISTAL beamline • Pump-probe diffraction: how ? • Pump-probe diffraction: motivations • Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 • Summary

  16. Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 [TPA (FeIII) TCC] PF6 [TPA (FeIII) TCC] Tris(2-pyridylméthyle) 3,4,5,6-tetrachlorocatecholate Lattice ↔ cooperative effects?

  17. Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 [TPA (FeIII) TCC] PF6 [TPA (FeIII) TCC] Tris(2-pyridylméthyle) 3,4,5,6-tetrachlorocatecholate Lattice ↔ cooperative effects? • Time-resolved structure determination at 180 K: <Fe-N> : fraction of molecules in the HS state Unit cell parameter a : elastic deformations Debye-Waller factor B: crystal temperature M. Lorenc et al., PRL 103 028301 (2009)

  18. Photoinduced effects in [TPA Fe(III) TPP] PF6: • Laser induced switching of molecules Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 [TPA (FeIII) TCC] PF6 [TPA (FeIII) TCC] Tris(2-pyridylméthyle) 3,4,5,6-tetrachlorocatecholate Lattice ↔ cooperative effects? • Time-resolved structure determination at 180 K: 1 <Fe-N> : fraction of molecules in the HS state Unit cell parameter a : elastic deformations Debye-Waller factor B: crystal temperature M. Lorenc et al., PRL 103 028301 (2009)

  19. Photoinduced effects in [TPA Fe(III) TPP] PF6: • Laser induced switching of molecules • Deformation wave propagation Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 [TPA (FeIII) TCC] PF6 [TPA (FeIII) TCC] Tris(2-pyridylméthyle) 3,4,5,6-tetrachlorocatecholate Lattice ↔ cooperative effects? • Time-resolved structure determination at 180 K: 1 2 <Fe-N> : fraction of molecules in the HS state Unit cell parameter a : elastic deformations Debye-Waller factor B: crystal temperature M. Lorenc et al., PRL 103 028301 (2009)

  20. Photoinduced effects in [TPA Fe(III) TPP] PF6: • Laser induced switching of molecules • Deformation wave propagation • Heat diffusion in the crystal Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 [TPA (FeIII) TCC] PF6 [TPA (FeIII) TCC] Tris(2-pyridylméthyle) 3,4,5,6-tetrachlorocatecholate Lattice ↔ cooperative effects? • Time-resolved structure determination at 180 K: 1 3 2 <Fe-N> : fraction of molecules in the HS state Unit cell parameter a : elastic deformations Debye-Waller factor B: crystal temperature M. Lorenc et al., PRL 103 028301 (2009)

  21. Photoinduced effects in [TPA Fe(III) TPP] PF6: • Laser induced switching of molecules • Deformation wave propagation • Heat diffusion in the crystal • Relaxation Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 [TPA (FeIII) TCC] PF6 [TPA (FeIII) TCC] Tris(2-pyridylméthyle) 3,4,5,6-tetrachlorocatecholate Lattice ↔ cooperative effects? • Time-resolved structure determination at 180 K: 1 3 4 2 <Fe-N> : fraction of molecules in the HS state Unit cell parameter a : elastic deformations Debye-Waller factor B: crystal temperature M. Lorenc et al., PRL 103 028301 (2009)

  22. Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 • Experimental setup

  23. kphi 002 kphi c X-rays Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 • Rocking curve measurements • Experimental setup Ewald sphere kphi-scan ↔ Imaging the 002 Bragg spot in 3D a c b Bragg spot extensions along a and b: Spread of (002) lattice plane tiltings in the a and b directions

  24. Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 ∑

  25. Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 ∑ ∑

  26. Test experiment: photoinduced effects in [TPA Fe(III) TCC] PF6 ∑ ∑ Two characteristic timescales: - Few 100 ns after excitation: peak broadening without profile change - Few µs after excitation: peak broadening with apparition of a tail Two lattice plane deformation cycles: - During step 2) propagation of deformation waves - During step 3) heat diffusion

  27. Summary • First time-resolved experiment at the CRISTAL beamline [ns resolution] • [TPA Fe(III) TCC] PF6: lattice plane deformations in laser-induced transient states • Improvement of the temporal resolution: - November 2011: reception of a fs laser → 70 ps resolution • - Year 2012: optimization of the low-alpha mode of operation • → 10 ps resolution • - Year 2014: « slicing » mode of operation • → 100 fs resolution Study of the interplays between lattice and electronic degrees of freedom Control of electronic properties in molecular crystals

  28. Sub-ps resolution: slicing • Time resolution ~ 100 fs Seminal paper : Zholents and Zolotorev, PRL 76 912 (1996) Available at Bessy, SLS, ALS 75fs bending magnet 70ps undulator 75fs wiggler Laser laser e-beam Laser pulse: 25 fs, few mJ 2.5 kHz, 800 nm bending magnet electron bunch (70 ps) electron bunch (75 fs) In the “sliced” zone, the electrons have energies spanning the range [E-ΔE ; E+ ΔE]. They will be spatially dispersed during their pass in the bending magnet. wiggler Exchange of energy between electrons and IR photons

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