Calibrating a spatially encoded time delay for transient absorption spectroscopy

Abstract

A novel spectroscopy termed single shot transient absorption (SSTA) is presented that can collect a transient absorption spectrum in 6 ms by using laser pulses with tilted wavefronts to spatially encode the delay between pump and probe pulse arrival times at the sample. The transient absorption technique determines the change in sample transmission that results from sample photoexcitation, and tracks this change as a function of the time delay between the arrival of the pump pulse and the probe pulse. Typically, these time delays are generated using a retroreflecting mirror mounted on a motorized translation stage, with a measurement collected at each translation stage position. Because these measurements must be performed in series, data collection requires a significant amount of time. This limits transient absorption to the measurement of systems that are static for the duration of the experiment. SSTA overcomes this restriction by employing pump and probe pulses which are each focused into a line and tilted with respect to each other to spatially encode time delays within the sample. Here, we describe the SSTA technique and instrumentation, demonstrate the principle of this spectroscopy, and present a method for calibrating the spatially encoded time delay by autocorrelation. This instrument will broaden the scop