Solid state core-exciton dynamics in NaCl observed by tabletop attosecond four-wave mixing spectroscopy
James D. Gaynor, Ashley P. Fidler, Yen-Cheng Lin, Hung-Tzu Chang, Michael Zuerch, Daniel M. Neumark, Stephen R. Leone
Abstract
Nonlinear wave mixing in solids with ultrafast x-rays can provide 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 ${\mathrm{Na}}^{+}$ ${L}_{2,3}$ edge core-excitons in NaCl around 33.5 eV. An inhomogeneous distribution of core-excitons underlying the well-known doublet absorption of the ${\mathrm{Na}}^{+}$ $\mathrm{\ensuremath{\Gamma}}$ 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. Approximately $<10\phantom{\rule{0.16em}{0ex}}\mathrm{fs}$ 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.