Time-resolved phase-sensitive second harmonic generation spectroscopy

Nowakowski, Paweł J.; Woods, David A.; Bain, Colin D.; Verlet, Jan R.R.

doi:10.1063/1.4909522

Time-resolved phase-sensitive second harmonic generation spectroscopy

Nowakowski, Paweł J.; Woods, David A.; Bain, Colin D.; Verlet, Jan R.R.

Authors

Paweł J. Nowakowski

David A. Woods

Professor Colin Bain c.d.bain@durham.ac.uk
Pro-Vice-Chancellor (Research)

Professor Jan Verlet j.r.r.verlet@durham.ac.uk
Professor

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.

Citation

Nowakowski, P. J., Woods, D. A., Bain, C. D., & Verlet, J. R. (2015). Time-resolved phase-sensitive second harmonic generation spectroscopy. The Journal of Chemical Physics, 142(8), https://doi.org/10.1063/1.4909522

Journal Article Type	Article
Acceptance Date	Feb 1, 2015
Online Publication Date	Feb 23, 2015
Publication Date	Feb 28, 2015
Deposit Date	Mar 19, 2015
Publicly Available Date	Mar 26, 2015
Journal	Journal of Chemical Physics
Print ISSN	0021-9606
Electronic ISSN	1089-7690
Publisher	American Institute of Physics
Peer Reviewed	Peer Reviewed
Volume	142
Issue	8
DOI	https://doi.org/10.1063/1.4909522

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Copyright 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 http://dx.doi.org/10.1063/1.4909522