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

[摘要] 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 nearinfrared (NIR) pulses characterizes the dynamics of the Na+ L-2,L-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. Approximately < 10 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.

[关键词] ABSORPTION;PHOTOEMISSION;ALKALI;SPECTRA;HALIDES