Coupled Valence Carrier and Core-Exciton Dynamics in WS$_{2}$ Probed by Few-Femtosecond Extreme Ultraviolet Transient Absorption Spectroscopy
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Coupled Valence Carrier and Core-Exciton Dynamics in WS$_{2}$ Probed by Few-Femtosecond Extreme Ultraviolet Transient Absorption Spectroscopy

  • Author(s): Chang, Hung-Tzu
  • Guggenmos, Alexander
  • Chen, Christopher T
  • Oh, Juwon
  • Géneaux, Romain
  • Chuang, Yi-De
  • Schwartzberg, Adam M
  • Aloni, Shaul
  • Neumark, Daniel M
  • Leone, Stephen R
  • et al.
Abstract

Few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy, performed with optical 500-1000 nm supercontinuum and broadband XUV pulses (30-50 eV), simultaneously probes dynamics of photoexcited carriers in WS$_{2}$ at the W O$_3$ edge (37-45 eV) and carrier-induced modifications of core-exciton absorption at the W N$_{6,7}$ edge (32-37 eV). Access to continuous core-to-conduction band absorption features and discrete core-exciton transitions in the same XUV spectral region in a semiconductor provides a novel means to investigate the effect of carrier excitation on core-exciton dynamics. The core-level transient absorption spectra, measured with either pulse arriving first to explore both core-level and valence carrier dynamics, reveal that core-exciton transitions are strongly influenced by the photoexcited carriers. A $1.2\pm0.3$ ps hole-phonon relaxation time and a $3.1\pm0.4$ ps carrier recombination time are extracted from the XUV transient absorption spectra from the core-to-conduction band transitions at the W O$_{3}$ edge. Global fitting of the transient absorption signal at the W N$_{6,7}$ edge yields $\sim 10$ fs coherence lifetimes of core-exciton states and reveals that the photoexcited carriers, which alter the electronic screening and band filling, are the dominant contributor to the spectral modifications of core-excitons and direct field-induced changes play a minor role. This work provides a first look at the modulations of core-exciton states by photoexcited carriers and advances our understanding of carrier dynamics in metal dichalcogenides.

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