Filtering noise in time and frequency domain for ultrafast pump-probe performed using low repetition rate lasers

Abstract

Optical pump-probe spectroscopy is a powerful tool to directly probe the carrier dynamics in materials down to sub-femtosecond resolution. To perform such measurements, while keeping the pump induced perturbation to the sample as small as possible, it is essential to have a detection scheme with a high signal to noise ratio. Achieving such a high signal to noise ratio is easy with phase sensitive detection based on a lock-in-amplifier when a high repetition rate laser is used as the optical pulse source. However, such a lock-in-amplifier based method does not work well when a low repetition rate laser is used for the measurement. In this article, a sensitive detection scheme, which combines the advantages of a boxcar that rejects noise in time domain and a lock-in-amplifier that isolates the signal in the frequency domain for performing pump-probe measurements using a low-repetition rate laser system, is proposed and experimentally demonstrated. A theoretical model to explain the process of signal detection and a method to reduce the pulse to pulse energy fluctuation in probe pulses is presented. By performing pump-probe measurements at various detection conditions, the optimum condition required for obtaining the transient absorption signal with low noise is presented. The reported technique is not limited to pump-probe measurements and can be easily modified to suit for other sensitive measurements at low repetition rates.