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- ItemUltrafast Structural Changes in Chiral Molecules Measured with Free-Electron Lasers(Bristol : IOP Publ., 2020) Schmidt, P.; Music, V.; Hartmann, G.; Boll, R.; Erk, B.; Bari, S.; Allum, F.; Baumann, T.M.; Brenner, G.; Brouard, M.; Burt, M.; Coffee, R.; Dörner, S.; Galler, A.; Grychtol, P.; Heathcote, D.; Inhester, L.; Kazemi, M.; Larsson, M.; Li, Z.; Lutmann, A.; Manschwetus, B.; Marder, L.; Mason, R.; Moeller, S.; Osipov, T.; Otto, H.; Passow, C.; Rolles, D.; Rupprecht, P.; Schubert, K.; Schwob, L.; Thomas, R.; Vallance, C.; Von Korff Schmising, C.; Wagner, R.; Walter, P.; Wolf, T.J.A.; Zhaunerchyk, V.; Meyer, M.; Ehresmann, A.; Knie, A.; Demekhin, P.V.; Ilchen, M.(X-ray) free-electron lasers are employed to site specifically interrogate atomic fragments during ultra-fast photolysis of chiral molecules via time-resolved photoelectron circular dichroism. © 2020 Institute of Physics Publishing. All rights reserved.
- ItemProbing nucleobase photoprotection with soft x-rays(Les Ulis : EDP Sciences, 2013) McFarland, B.K.; Farrell, J.P.; Berrah, N.; Bostedt, C.; Bozek, J.; Bucksbaum, P.H.; Coffee, R.; Cryan, J.; Fang, L.; Feifel, R.; Gaffney, K.; Glownia, J.; Martinez, T.; Mucke, M.; Murphy, B.; Miyabe, S.; Natan, A.; Osipov, T.; Petrovic, V.; Schorb, S.; Schultz, T.; Spector, L.; Tarantelli, F.; Tenney, I.; Wang, S.; White, W.; White, J.; Gühr, M.Nucleobases absorb strongly in the ultraviolet region, leading to molecular excitation into reactive states. The molecules avoid the photoreactions by funnelling the electronic energy into less reactive states on an ultrafast timescale via non-Born-Oppenheimer dynamics. Current theory on the nucleobase thymine discusses two conflicting pathways for the photoprotective dynamics. We present our first results of our free electron laser based UV-pump soft x-ray-probe study of the photoprotection mechanism of thymine. We use the high spatial sensitivity of the Auger electrons emitted after the soft x-ray pulse induced core ionization. Our transient spetra show two timescales on the order of 200 fs and 5 ps, in agreement with previous (all UV) ultrafast experiments. The timescales appear at different Auger kinetic energies which will help us to decipher the molecular dynamics.
- ItemImaging molecular structure through femtosecond photoelectron diffraction on aligned and oriented gas-phase molecules(Cambridge [u.a.] : Royal Society of Chemistry, 2014) Boll, R.; Rouzée, A.; Adolph, M.; Anielski, D.; Aquila, A.; Bari, S.; Bomme, C.; Bostedt, C.; Bozek, J.D.; Chapman, H.N.; Christensen, L.; Coffee, R.; Coppola, N.; De, S.; Decleva, P.; Epp, S.W.; Erk, B.; Filsinger, F.; Foucar, L.; Gorkhover, T.; Gumprecht, L.; Hömke, A.; Holmegaard, L.; Johnsson, P.; Kienitz, J.S.; Kierspel, T.; Krasniqi, F.; Kühnel, K.-U.; Maurer, J.; Messerschmidt, M.; Moshammer, R.; Müller, N.L.M.; Rudek, B.; Savelyev, E.; Schlichting, I.; Schmidt, C.; Scholz, F.; Schorb, S.; Schulz, J.; Seltmann, J.; Stener, M.; Stern, S.; Techert, S.; Thøgersen, J.; Trippel, S.; Viefhaus, J.; Vrakking, M.; Stapelfeldt, H.; Küpper, J.; Ullrich, J.; Rudenko, A.; Rolles, D.This paper gives an account of our progress towards performing femtosecond time-resolved photoelectron diffraction on gas-phase molecules in a pump-probe setup combining optical lasers and an X-ray free-electron laser. We present results of two experiments aimed at measuring photoelectron angular distributions of laser-aligned 1-ethynyl-4-fluorobenzene (C8H5F) and dissociating, laser-aligned 1,4-dibromobenzene (C6H4Br2) molecules and discuss them in the larger context of photoelectron diffraction on gas-phase molecules. We also show how the strong nanosecond laser pulse used for adiabatically laser-aligning the molecules influences the measured electron and ion spectra and angular distributions, and discuss how this may affect the outcome of future time-resolved photoelectron diffraction experiments.