Rapid scan white light pump–probe spectroscopy with 100 kHz shot-to-shot detection

Abstract

We demonstrate a femtosecond pump–probe spectrometer that utilizes a white light supercontinuum as input and relies on mutual synchronization of the laser repetition rate, acousto-optical chopper, pump–probe delay stage, and the CCD camera to record shot-to-shot pump–probe spectra while the pump–probe delay is scanned synchronously with the laser repetition rate. The unique combination of technologies implemented here allows for electronically controllable and repetition-rate scalable detection throughput that is only limited by the camera frame rate. Despite high probe RMS fluctuations due to sample scatter (from ∼1.8% with solvent to 7.9% with sample scatter), a combination of fast and slow averaging with a fine sampling of pump–probe delay leads to reduction of RMS noise without multichannel referencing down to ∼0.4 mOD for a scattering nanotube sample. Throughput and limitations of the rapid versus stepwise scanning approaches are analyzed. Experimental comparison with stepwise scan shows ∼1.9x noise reduction in a significantly faster experiment, suggesting an additional suppression of 1/f noise enabled by rapid scan data collection. The particular combination of technologies implemented here makes our approach especially suitable for high throughput impulsive pump–probe micro-spectroscopy of highly scattering samples, without added cost and complexity of light sources, multichannel detection, or long sample exposure.