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Time-resolved phase-sensitive second harmonic generation spectroscopy.

Nowakowski, Paweł J. and Woods, David A. and Bain, Colin D. and Verlet, Jan R. R. (2015) 'Time-resolved phase-sensitive second harmonic generation spectroscopy.', Journal of chemical physics., 142 (8). 084201.


A methodology based on time-resolved, phase-sensitive second harmonic generation (SHG) for probing the excited state dynamics of species at interfaces is presented. It is based on an interference measurement between the SHG from the sample and a local oscillator generated at a reference together with a lock-in measurement to remove the large constant offset from the interference. The technique is characterized by measuring the phase and excited state dynamics of the dye malachite green at the water/air interface. The key attributes of the technique are that the observed signal is directly proportional to sample concentration, in contrast to the quadratic dependence from non-phase sensitive SHG, and that the real and imaginary parts of the 2nd order non-linear susceptibility can be determined independently. We show that the method is highly sensitive and can provide high quality excited state dynamics in short data acquisition times.

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Publisher statement:© 2015 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 Journal of Chemical Physics, 142, 084201 (2015) and may be found at
Date accepted:01 February 2015
Date deposited:26 March 2015
Date of first online publication:23 February 2015
Date first made open access:No date available

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