Solid-state core-exciton dynamics in NaCl observed by tabletop attosecond four-wave mixing spectroscopy

TL;DR

This paper demonstrates tabletop attosecond four-wave mixing spectroscopy to study core-exciton dynamics in NaCl, revealing ultrafast coherence and complex electronic interactions in solid-state materials.

Contribution

It introduces a novel tabletop method for time-resolved solid-state spectroscopy using attosecond XUV four-wave mixing to probe core-excitons.

Findings

Deconvoluted inhomogeneous core-exciton distribution

Observed sub-10 femtosecond coherence lifetimes

Characterized dark excitonic states and their couplings

Abstract

Nonlinear wave-mixing in solids with ultrafast x-rays can provide new insight into complex electronic dynamics of materials. Here, tabletop-based attosecond noncollinear four-wave mixing (FWM) spectroscopy using one extreme ultraviolet (XUV) pulse from high harmonic generation and two separately timed few-cycle near-infrared (NIR) pulses characterizes the dynamics of the Na+ L2,3 edge core-excitons in NaCl around 33.5 eV. An inhomogeneous distribution of core-excitons underlying the well-known doublet absorption of the Na+ \Gamma-point core-exciton spectrum is deconvoluted by the resonance-enhanced nonlinear wave-mixing spectroscopy. In addition, other dark excitonic states that are coupled to the XUV-allowed levels by the NIR pulses are characterized spectrally and temporally. Approximate sub-10 femtosecond coherence lifetimes of the core-exciton states are observed. The core-excitonic properties are discussed in the context of strong electron-hole exchange interactions, electron-electron correlation, and electron-phonon broadening. This investigation successfully indicates that tabletop attosecond FWM spectroscopies represent a viable technique for time-resolved solid-state measurements.