Rapid Scan White Light Two-dimensional Electronic Spectroscopy with 100 kHz Shot-to-Shot Detection

Abstract: We demonstrate an approach to two-dimensional electronic spectroscopy (2DES) that combines the benefits of shot-to-shot detection at high-repetition rates with the simplicity of a broadband white light continuum input and conventional optical elements to generate phase-locked pump pulse pairs. We demonstrate this through mutual synchronization between the laser repetition rate, acousto-optical deflector (AOD), pump delay stage and the CCD line camera, which allows rapid scanning of pump optical delay synchronously with the laser repetition rate while the delay stage is moved at a constant velocity. The resulting shot-to-shot detection scheme is repetition rate scalable and only limited by the CCD line rate and the maximum stage velocity. Using this approach, we demonstrate measurement of an averaged 2DES absorptive spectrum in as much as 1.2 seconds of continuous sample exposure per 2D spectrum. We achieve a signal-to-noise ratio (SNR) of 6.8 for optical densities down to 0.05 with 11.6 seconds of averaging at 100 kHz laser repetition rate. Combining rapid scanning of mechanical delay lines with shot-to-shot detection as demonstrated here provides a viable alternative to acousto-optic pulse shaping (AOPS) approaches that is repetition-rate scalable, has comparable throughput and sensitivity, and minimizes sample exposure per 2D spectrum with promising micro-spectroscopy applications.