A time-resolved, phase-sensitive second harmonic generation (SHG) method to probe the excited state dynamics of interfacial species is presented. It is based on an interference measurement between the SHG from a sample and a local oscillator generated at a reference surface in which an entire interference pattern is recorded in a single shot by using a spatially varying phase unit comprised of a pair of wedges that sandwich the reference sample. In combination with 30 kHz modulation of the experiment, shot-to-shot pump-probe measurements are presented. The technique is characterised by measuring the time-resolved change in the amplitude and phase of the interference pattern due to the excited state dynamics of the dye malachite green at the air/water interface. The key attributes of the technique are its excellent phase stability and sensitivity, and relatively short data acquisition times.
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Research Article| November 28 2018
Time-resolved second harmonic generation with single-shot phase sensitivity
Alexandra L. Tyson;
David A. Woods;
Alexandra L. Tyson, David A. Woods, Jan R. R. Verlet; Time-resolved second harmonic generation with single-shot phase sensitivity. J. Chem. Phys. 28 November 2018; 149 (20): 204201. https://doi.org/10.1063/1.5061817
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