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- ItemExcited-state relaxation of hydrated thymine and thymidine measured by liquid-jet photoelectron spectroscopy: experiment and simulation(Washington, DC : ACS Publications, 2015) Buchner, Franziska; Nakayama, Akira; Yamazaki, Shohei; Ritze, Hans-Hermann; Lübcke, AndreaTime-resolved photoelectron spectroscopy is performed on thymine and thymidine in aqueous solution to study the excited-state relaxation dynamics of these molecules. We find two contributions with sub-ps lifetimes in line with recent excited-state QM/MM molecular dynamics simulations (J. Chem. Phys.2013, 139, 214304). The temporal evolution of ionization energies for the excited ππ* state along the QM/MM molecular dynamics trajectories were calculated and are compatible with experimental results, where the two contributions correspond to the relaxation paths in the ππ* state involving different conical intersections with the ground state. Theoretical calculations also show that ionization from the nπ* state is possible at the given photon energies, but we have not found any experimental indication for signal from the nπ* state. In contrast to currently accepted relaxation mechanisms, we suggest that the nπ* state is not involved in the relaxation process of thymine in aqueous solution.
- ItemHigh-order parametric generation of coherent XUV radiation(Washington, DC : Soc., 2021) Hort, O.; Dubrouil, A.; Khokhlova, M.A.; Descamps, D.; Petit, S.; Burgy, F.; Mével, E.; Constant, E.; Strelkov, V.V.Extreme ultraviolet (XUV) radiation finds numerous applications in spectroscopy. When the XUV light is generated via high-order harmonic generation (HHG), it may be produced in the form of attosecond pulses, allowing access to unprecedented ultrafast phenomena. However, the HHG efficiency remains limited. Here we present an observation of a new regime of coherent XUV emission which has a potential to provide higher XUV intensity, vital for applications. We explain the process by high-order parametric generation, involving the combined emission of THz and XUV photons, where the phase matching is very robust against ionization. This introduces a way to use higher-energy driving pulses, thus generating more XUV photons.
- ItemDisparate ultrafast dynamics of itinerant and localized magnetic moments in gadolinium metal([London] : Nature Publishing Group UK, 2015) Frietsch, B.; Bowlan, J.; Carley, R.; Teichmann, M.; Wienholdt, S.; Hinzke, D.; Nowak, U.; Carva, K.; Oppeneer, P. M.; Weinelt, M.The Heisenberg–Dirac intra-atomic exchange coupling is responsible for the formation of the atomic spin moment and thus the strongest interaction in magnetism. Therefore, it is generally assumed that intra-atomic exchange leads to a quasi-instantaneous aligning process in the magnetic moment dynamics of spins in separate, on-site atomic orbitals. Following ultrashort optical excitation of gadolinium metal, we concurrently record in photoemission the 4f magnetic linear dichroism and 5d exchange splitting. Their dynamics differ by one order of magnitude, with decay constants of 14 versus 0.8 ps, respectively. Spin dynamics simulations based on an orbital-resolved Heisenberg Hamiltonian combined with first-principles calculations explain the particular dynamics of 5d and 4f spin moments well, and corroborate that the 5d exchange splitting traces closely the 5d spin-moment dynamics. Thus gadolinium shows disparate dynamics of the localized 4f and the itinerant 5d spin moments, demonstrating a breakdown of their intra-atomic exchange alignment on a picosecond timescale.
- ItemRaman gas self-organizing into deep nano-trap lattice([London] : Nature Publishing Group UK, 2016) Alharbi, M.; Husakou, A.; Chafer, M.; Debord, B.; Gérôme, F.; Benabid, F.Trapping or cooling molecules has rallied a long-standing effort for its impact in exploring new frontiers in physics and in finding new phase of matter for quantum technologies. Here we demonstrate a system for light-trapping molecules and stimulated Raman scattering based on optically self-nanostructured molecular hydrogen in hollow-core photonic crystal fibre. A lattice is formed by a periodic and ultra-deep potential caused by a spatially modulated Raman saturation, where Raman-active molecules are strongly localized in a one-dimensional array of nanometre-wide sections. Only these trapped molecules participate in stimulated Raman scattering, generating high-power forward and backward Stokes continuous-wave laser radiation in the Lamb-Dicke regime with sub-Doppler emission spectrum. The spectrum exhibits a central line with a sub-recoil linewidth as low as ∼14 kHz, more than five orders of magnitude narrower than conventional-Raman pressure-broadened linewidth, and sidebands comprising Mollow triplet, motional sidebands and four-wave mixing.
- ItemX-ray imaging of chemically active valence electrons during a pericyclic reaction(London : Nature Publishing Group, 2014) Bredtmann, T.; Ivanov, M.; Dixit, G.Time-resolved imaging of chemically active valence electron densities is a long-sought goal, as these electrons dictate the course of chemical reactions. However, X-ray scattering is always dominated by the core and inert valence electrons, making time-resolved X-ray imaging of chemically active valence electron densities extremely challenging. Here we demonstrate an effective and robust method, which emphasizes the information encoded in weakly scattered photons, to image chemically active valence electron densities. The degenerate Cope rearrangement of semibullvalene, a pericyclic reaction, is used as an example to visually illustrate our approach. Our work also provides experimental access to the long-standing problem of synchronous versus asynchronous bond formation and breaking during pericyclic reactions.