Narrowband nonlinear optical spectroscopy with spatially chirped broadband pulses.

Abstract

Nonlinear optical vibrational spectroscopies are powerful experimental tools for inspecting material properties that are difficult to acquire otherwise. As ultrafast lasers used in such experiments are typically of much broader bandwidth than vibrational modes, narrowband filtering is usually essential, and the utility of laser energy is often highly inefficient. Here we introduce an experimental scheme to break this trade-off. A broadband beam is spatially chirped as it reaches the sample, and generates sum-frequency signals upon overlapping with another broadband, unchirped beam. A narrowband spectrum can then be retrieved from the spatially dispersed image of signals, with both broadband pulses fully utilized. The scheme is also readily employed as a spatially resolved spectroscopy technique without scanning, and can be easily extended to other wave-mixing experiments.