2014
DOI: 10.1364/ol.39.004274
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Heterodyne-detected and ultrafast time-resolved second-harmonic generation for sensitive measurements of charge transfer

Abstract: In organic photovoltaics many key ultrafast processes occur at the interface between electron donor and acceptor molecules. Traditional ultrafast spectroscopies, such as pump-probe or time-resolved fluorescence, are not ideal for studying the interface because most of their signal is from the bulk material. Time-resolved second-harmonic generation (TRSHG) spectroscopy solves this problem by only generating signal from the interface. We demonstrate an optically heterodyned TRSHG to reduce the impact of stray li… Show more

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Cited by 11 publications
(18 citation statements)
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“…To probe only the water/air interface, we employ phase-sensitive SHG. Phase-sensitive SHG has been used both nonspectroscopically and spectroscopically, , and recently, a number of groups have combined this into time-resolved and phase-sensitive SHG, primarily for use at semiconductor interfaces. We have developed a variant of these techniques that is not spectroscopic but benefits from a lock-in measurement and excellent phase stability, which is crucial to the current measurements .…”
mentioning
confidence: 99%
“…To probe only the water/air interface, we employ phase-sensitive SHG. Phase-sensitive SHG has been used both nonspectroscopically and spectroscopically, , and recently, a number of groups have combined this into time-resolved and phase-sensitive SHG, primarily for use at semiconductor interfaces. We have developed a variant of these techniques that is not spectroscopic but benefits from a lock-in measurement and excellent phase stability, which is crucial to the current measurements .…”
mentioning
confidence: 99%
“…Simple experimental corrections, such as using larger spot sizes or shorter pulse durations, can be used to preserve the same sample fluence (and avoid sample damage) while yielding more SHG photons per laser shot. For small samples and systems employing high numerical aperture objective optics, this solution may not be practical, meaning schemes employing heterodyne detection 21,22 or stimulated SHG 23 should be investigated. Such optical signal amplification techniques will allow for measurement of additional signal components that are buried in the noise and difficult to resolve, with the primary limitations being the number of demodulators that simultaneously analyze the signal.…”
Section: Discussionmentioning
confidence: 99%
“…The pump and probe pulse durations estimated from the SPEAR [113] and MIIPS [114] pulse compression algorithms were 12.8fs and 10.0fs, respectively.…”
Section: Brc 2des Experimentsmentioning
confidence: 99%