Abstract
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 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 resonance of nitric oxide (NO), and excited state neutral molecules are probed with a time-delayed UV laser pulse.
- Received 10 February 2020
- Revised 21 May 2020
- Accepted 9 July 2020
DOI:https://doi.org/10.1103/PhysRevLett.125.073203
© 2020 American Physical Society
Physics Subject Headings (PhySH)
synopsis
Jumpstarting Electron Motion in Molecules
Published 11 August 2020
Ultrashort pulses of x rays swap electrons around in molecules of nitric oxide, an important first step to tracking charge motion in molecules.
See more in Physics