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Time-resolved second harmonic generation with single-shot phase sensitivity.

Tyson, Alexandra L. and Woods, David A. and Verlet, Jan R. R. (2018) 'Time-resolved second harmonic generation with single-shot phase sensitivity.', Journal of chemical physics., 149 (20). p. 204201.


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.

Item Type:Article
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Publisher statement:© 2018 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics. The following article appeared in Tyson, Alexandra L., Woods, David A. & Verlet, Jan R. R. (2018). Time-resolved second harmonic generation with single-shot phase sensitivity. The Journal of Chemical Physics 149(20): 204201 and may be found at
Date accepted:02 November 2018
Date deposited:07 December 2018
Date of first online publication:28 November 2018
Date first made open access:28 November 2019

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