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Purely absorptive three-dimensional infrared spectroscopy


Garrett-Roe, S; Hamm, P (2009). Purely absorptive three-dimensional infrared spectroscopy. Journal of Chemical Physics, 130(16):164510.

Abstract

We demonstrate a method to collect purely absorptive three-dimensional (3D) fifth-order vibrational spectra on the model system CO2 in H2O. The six beam interferometer is described, as well as a method to experimentally determine the phase of the 3D spectrum. The measured spectra agree very well with simulations of the data based on the cumulant expansion. There are five peaks corresponding to different paths up and down the vibrational ladder. The positions, signs, and amplitudes of the peaks agree with theoretical predictions, and the intensities of the peaks scale linearly with concentration. Based on the concentration dependence and agreement between the simulations and measurements, we conclude that cascaded lower order signals contribute negligibly to the observed signal.

We demonstrate a method to collect purely absorptive three-dimensional (3D) fifth-order vibrational spectra on the model system CO2 in H2O. The six beam interferometer is described, as well as a method to experimentally determine the phase of the 3D spectrum. The measured spectra agree very well with simulations of the data based on the cumulant expansion. There are five peaks corresponding to different paths up and down the vibrational ladder. The positions, signs, and amplitudes of the peaks agree with theoretical predictions, and the intensities of the peaks scale linearly with concentration. Based on the concentration dependence and agreement between the simulations and measurements, we conclude that cascaded lower order signals contribute negligibly to the observed signal.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Language:English
Date:24 April 2009
Deposited On:26 Jun 2009 11:21
Last Modified:20 May 2016 09:32
Publisher:American Institute of Physics
ISSN:0021-9606
Funders:Swiss National Science Foundation (SNF)
Additional Information:©2009 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 'The Journal of Chemical Physics' and may be found at http://link.aip.org/link/?JCPSA6/130/164510/1
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:10.1063/1.3122982
PubMed ID:19405597
Permanent URL: http://doi.org/10.5167/uzh-19292

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