All-Optical Field-Resolved Spectroscopy With Interferometric Nonlinear Cross-Correlations

Direct time-domain measurements of electric fields enable sub-cycle spectroscopy of light-matter interactions, but established techniques such as electro-optic sampling are constrained in their bandwidth by gate-pulse duration and phase-matching limitations. Alternative approaches have emerged in recent years based on asymmetric interferometric nonlinear cross-correlations with highly nonlinear media, and have demonstrated, for example, the field-resolved study of exciton ensembles. However, these nonlinear cross-correlation-based techniques have been benchmarked almost exclusively by self-referenced pulse characterization rather than by their quantitative spectroscopic performance, and all-optical approaches have received less attention than those based on direct charge emission. Here we extend all-optical asymmetric interferometric cross-correlation to higher nonlinearities in sub-wavelength films and demonstrate field-resolved spectroscopy of the free-induction decay of two ro-vibrational bands of ambient water vapor with a performance comparable to state of the art electro-optic sampling. The measurement spans 190 THz of bandwidth (80 THz to 270 THz) with sub-500 GHz spectral resolution, a spectral intensity dynamic range of six orders of magnitude, and a field-strength noise floor of 100 kV per meter. We anticipate the rapid adoption of here presented all-optical sampling to many experimental settings and a broad impact beyond the ultrafast optics research community as it is drastically simplified in comparison to ionization based techniques and allows the translation of electro-optic-sampling-level sensitivity into higher frequency ranges not previously accessible by conventional tools.