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Electronic Population Transfer via Impulsive Stimulated X-Ray Raman Scattering with Attosecond Soft-X-Ray Pulses

Jordan T. O'Neal, Elio G. Champenois, Solène Oberli, Razib Obaid, Andre Al-Haddad, Jonathan Barnard, Nora Berrah, Ryan Coffee, Joseph Duris, Gediminas Galinis, Douglas Garratt, James M. Glownia (+17 others)
2020 Physical Review Letters  
Free-electron lasers provide a source of x-ray pulses short enough and intense enough to drive nonlinearities in molecular systems. Impulsive interactions driven by these x-ray pulses provide a way to create and probe valence electron motions with high temporal and spatial resolution. Observing these electronic motions is crucial to understand the role of electronic coherence in chemical processes. A simple nonlinear technique for probing electronic motion, impulsive stimulated x-ray Raman
more » ... ed x-ray Raman scattering (ISXRS), involves a single impulsive interaction to produce a coherent superposition of electronic states. We demonstrate electronic population transfer via ISXRS using broad bandwidth (5.5 eV full width at half maximum) attosecond x-ray pulses produced by the Linac Coherent Light Source. The impulsive excitation is resonantly enhanced by the oxygen 1s→2π^{*} resonance of nitric oxide (NO), and excited state neutral molecules are probed with a time-delayed UV laser pulse.
doi:10.1103/physrevlett.125.073203 pmid:32857563 fatcat:kdzdzvz5rzdvlonvhzlih5phti