Femtosecond core level photoemision spectroscopy on 1T-TaS2 using 60 eV laser source

TL;DR

This study demonstrates femtosecond core-level photoemission spectroscopy on 1T-TaS2 using a 60 eV laser source, revealing ultrafast charge-density-wave dynamics and collective excitations at the atomic level.

Contribution

It introduces a high-intensity 60 eV laser source for time-resolved core-level photoemission spectroscopy, enabling real-time, site-specific observation of electronic dynamics in 1T-TaS2.

Findings

Ultrafast melting and recovery of charge-density-wave amplitude.

Observation of long-lived oscillations indicating collective amplitudon excitations.

Transfer of 0.01 electrons among Ta atoms during dynamics.

Abstract

Time-resolved photoelectron spectroscopy (trPES) can directly detect transient electronic structure, thus bringing out its promising potential to clarify nonequilibrium processes arising in condensed matters. Here we report the result of core-level (CL) trPES on 1T-TaS2, realized by developing a high-intensity 60 eV laser obtained by high-order harmonic (HH) generation. Ta4f CL-trPES offers the transient amplitude of the charge-density-wave (CDW), via the site-selective and real-time observation of Ta electrons. The present result indicates an ultrafast photoinduced melting and recovery of CDW amplitude, followed by a peculiar long-life oscillation (i.e. collective amplitudon excitation) accompanying the transfer of 0.01 electrons among adjacent Ta atoms. CL-trPES offers a broad range of opportunities for investigating the ultrafast atom-specific electron dynamics in photo-related phenomena of interest.