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

Jordan T. O’Neal et al.
Phys. Rev. Lett. 125, 073203 – Published 11 August 2020
Physics logo See synopsis: Jumpstarting Electron Motion in Molecules
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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 1s2π* resonance of nitric oxide (NO), and excited state neutral molecules are probed with a time-delayed UV laser pulse.

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  • 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)

Nonlinear DynamicsAtomic, Molecular & Optical

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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.

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Vol. 125, Iss. 7 — 14 August 2020

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