Time-resolved phase-sensitive second harmonic generation spectroscopy

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

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
• Public URL: https://durham-repository.worktribe.com/output/1413309