Abstract

We propose a scheme for probing the structure of vibrating molecules with photoelectrons generated from ultrashort soft-x-ray pulses. As an example we analyze below-100-eV photoelectrons liberated from the S(2p) orbital of vibrating SF₆ molecules to image very small structural changes of molecular vibration. In particular, photoionization cross sections and photoelectron angular distributions (PAD) at nonequilibrium geometries can be retrieved accurately with photoelectrons near the shape resonance at 13 eV. This is achieved with a pump-probe scheme, in which the symmetric stretch mode is first Raman excited predominantly by a relatively short laser pulse and then later probed at different time delays by a few-femtosecond soft-x-ray pulse with photon energy near 200 eV.

Department(s)

Physics

Keywords and Phrases

Molecules; Optical Pumping; Photoelectrons; Photoionization; Pumping (Laser); Sulfur Hexafluoride; Time Delay; Vibration Analysis, Non Equilibrium; Photoelectron Angular Distributions; Photoionization Cross Section; Pump-Probe Scheme; Shape Resonance; Short Laser Pulse; Soft X Ray Pulse; Vibrating Molecules, Photons

International Standard Serial Number (ISSN)

2469-9926

Document Type

Article - Journal

Document Version

Final Version

File Type

text

Language(s)

English

Rights

© 2016 American Physical Society (APS), All rights reserved.

Included in

Physics Commons

Share

 
COinS