Widefield pump-probe microscopy with coherent background subtraction by angle-compensated temporal shearing

Abstract: Pump-probe microscopy enables label-free imaging of structural and chemical features of samples. However, signals in pump-probe microscopy are typically small and often must be measured in the presence of large backgrounds. As a result, achieving measurements with a high signal-to-noise ratio is challenging, particularly when using sensors that are easily saturated, such as CMOS cameras. We present a method for enhancing signal-to-noise ratio while avoiding detector saturation. In this approach, temporally separated (sheared) reference and probe pulses transmit through a sample before and after the arrival of a pump pulse. The probe and reference pulses are then temporally recombined with opposing phases and nearly matched amplitudes, resulting in interferometric background subtraction. This recombining operation is performed by a novel common-path interferometer. Unlike previous techniques for temporal shearing, this interferometer demonstrates negligible phase and group delay dispersion with angle of incidence, allowing convenient widefield imaging. To our knowledge, this is the first common-path interferometer with such a property. We demonstrate the technique by measuring transient absorption signals in gold nanorod films with a signal-to-background ratio enhanced by over 100% and a signal-to-noise ratio enhanced by about 70%.