Time-resolved phase-sensitive second harmonic generation spectroscopy

The Journal of Chemical Physics
Paweł J NowakowskiJan R R Verlet

Abstract

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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Citations

Oct 10, 2015·The Journal of Chemical Physics·Matthias J Hofmann, Patrick Koelsch
Dec 14, 2016·Nature Communications·Paul E OhnoKenneth B Eisenthal
Dec 7, 2018·The Journal of Chemical Physics·Alexandra L TysonJan R R Verlet
Jun 11, 2021·The Journal of Physical Chemistry Letters·Emily MaFranz M Geiger
Apr 23, 2019·The Journal of Physical Chemistry Letters·Paul E OhnoFranz M Geiger
Sep 30, 2016·The Journal of Physical Chemistry Letters·Paweł J NowakowskiJan R R Verlet

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