Open AccessTime-resolved phase-sensitive second harmonic generation spectroscopy
Author(s) -
Paweł Nowakowski,
David A. Woods,
Colin D. Bain,
Jan R. R. Verlet
Publication year - 2015
Publication title -
the journal of chemical physics
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.071
H-Index - 357
eISSN - 1089-7690
pISSN - 0021-9606
DOI - 10.1063/1.4909522
Subject(s) - excited state , malachite green , second harmonic generation , spectroscopy , phase (matter) , offset (computer science) , materials science , optics , quadratic equation , interference (communication) , analytical chemistry (journal) , atomic physics , physics , chemistry , laser , telecommunications , computer science , mathematics , quantum mechanics , organic chemistry , adsorption , chromatography , programming language , channel (broadcasting) , geometry
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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