Optimizing pump-probe reflectivity measurements of ultrafast photoacoustics with modulated asynchronous optical sampling.

Time-resolved optical pump-probe experiments enable the study of complex light-matter interactions on ultrafast timescales, provided that they reach sufficient sensitivity. For instance, with pump-induced ultrafast photoacoustics, probing the typically small changes in optical properties requires a high signal-to-noise ratio. Asynchronous optical sampling (ASOPS), using two separate pulsed lasers at slightly different repetition rates, can be effective at removing noise by averaging many rapidly acquired traces. However, the pump-probe delay scan with ASOPS is always as long as the pump pulse interval, which is inefficient if the delay-time range of interest is shorter. Here, we demonstrate two modified ASOPS schemes that optimize measurement efficiency by only scanning the range of interest. The modification based on frequency modulated ASOPS (MASOPS) is most efficient, especially in the presence of low-frequency flicker noise. We provide a proof-of-concept measurement of ultrafast photoacoustics in which we use MASOPS to scan a time delay of 1/20 of the pump pulse interval. The resulting noise floor is 20 times lower compared to conventional ASOPS, allowing for 20 times faster measurements. Furthermore, we show that by taking experimental noise characteristics into account, more traditional pump-probe methods can also be optimized.