Probing ultrafast molecular dynamics in O$_{2}$ using XUV/IR pump-probe studies

ORAL

Abstract

We investigate the molecular dynamics via different dissociative and autoionizing pathways in molecular oxygen using a pump-probe scheme with ultrashort extreme ultraviolet (XUV) laser pulses. Our primary focus is to study the molecular dynamics in the superexcited Rydberg states in a time-resolved manner. The O$_{2}$ molecules are pumped by 20.2 eV and 23.1 eV XUV pulses (13$^{\mathrm{th}}$ and 15$^{\mathrm{th}}$ harmonics). Probing the relaxation dynamics with an infrared (IR) pulse at very long delays (100s of fs) enables us to measure the lifetimes of these Rydberg states. We also observe an enhancement and suppression of vibrational levels of the O$_{2}^{+}$ ion due to the presence of IR. The high flux XUV pulses used for this experiment are generated in an Ar gas by IR pulses from our state-of-the-art 30 mJ, 50 Hz laser system. The pulses are overlapped with the supersonic jet in our Momentum Imaging for TimE Resolved Studies (MISTERS) setup. The cold target in our setup, combined with a very tight focussing geometry and a 3D momentum detection capability gives a high kinetic energy resolution. Molecular dynamics in other polyatomic molecules are also under investigation.

*Chemical Sciences Division, Lawrence Berkeley National Laboratory

Authors

  • D. Ray

    • Chemical Sciences Division, Lawrence Berkeley National Laboratory
  • F.P. Sturm

    • Chemical Sciences Division, Lawrence Berkeley National Laboratory
  • T.W. Wright

    • Chemical Sciences Division, Lawrence Berkeley National Laboratory
  • P. Ranitovic

    • Chemical Sciences Division, Lawrence Berkeley National Laboratory
  • N.H. Shivaram

    • Chemical Sciences Division, Lawrence Berkeley National Laboratory
  • I. Bocharova

    • Chemical Sciences Division, Lawrence Berkeley National Laboratory
  • A. Belkacem

    • Chemical Sciences Division, Lawrence Berkeley National Laboratory
  • Th. Weber

    • Chemical Sciences Division, Lawrence Berkeley National Laboratory