O'Neal, Jordan T.Champenois, Elio G.Oberli, SoleneObaid, RazibAl-Haddad, AndreBarnard, JonathanBerrah, NoraCoffee, RyanDuris, JosephGalinis, GediminasGarratt, DouglasGlownia, James M.Haxton, DanielHo, PhayLi, SiqiLi, XiangMacArthur, JamesMarangos, Jon P.Natan, AdiShivaram, NiranjanSlaughter, Daniel S.Walter, PeterWandel, ScottYoung, LindaBostedt, ChristophBucksbaum, Philip H.Picon, AntonioMarinelli, AgostinoCryan, James P.2020-08-262020-08-262020-08-262020-08-1110.1103/PhysRevLett.125.073203https://infoscience.epfl.ch/handle/20.500.14299/171135WOS:000558086800003Free-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 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 -> 2 pi* resonance of nitric oxide (NO), and excited state neutral molecules are probed with a time-delayed UV laser pulse.Physics, MultidisciplinaryPhysicshigh-resolutionbuilding-blocknitric-oxidespectroscopyphotoionizationmoleculesdynamicsatomsnotext::journal::journal article::research article