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Intrinsic phasing of heterodyne-detected multidimensional infrared spectra


Johnson, Philip J M; Koziol, Klemens L; Hamm, Peter (2017). Intrinsic phasing of heterodyne-detected multidimensional infrared spectra. Optics Express, 25(3):2928.

Abstract

We show that it is possible to phase multidimensional infrared spectra generated by a boxcars geometry four-wave mixing spectrometer directly from the signal generated by the molecular vibration of interest, without the need for auxiliary phasing measurements. For isolated vibrations, the phase profile of the 2D response smoothly varies between fixed phase limits, allowing for a general target for phasing independent of the degree of anharmonicity exhibited between the ground and excited state. As a proof of principle, the 2D response of the similar to 2155 cm(-1) thiocyanate stretch vibration of MeSCN, a system exhibiting anharmonicity such that the 0-1 and 1-2 transitions are spectrally isolated, is successfuly phased directly from the experimental spectra. The methodology is also applied to correctly phase extremely weak signals of the unnatural amino acid azidohomoalanine following background subtraction.

Abstract

We show that it is possible to phase multidimensional infrared spectra generated by a boxcars geometry four-wave mixing spectrometer directly from the signal generated by the molecular vibration of interest, without the need for auxiliary phasing measurements. For isolated vibrations, the phase profile of the 2D response smoothly varies between fixed phase limits, allowing for a general target for phasing independent of the degree of anharmonicity exhibited between the ground and excited state. As a proof of principle, the 2D response of the similar to 2155 cm(-1) thiocyanate stretch vibration of MeSCN, a system exhibiting anharmonicity such that the 0-1 and 1-2 transitions are spectrally isolated, is successfuly phased directly from the experimental spectra. The methodology is also applied to correctly phase extremely weak signals of the unnatural amino acid azidohomoalanine following background subtraction.

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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:6 February 2017
Deposited On:09 Mar 2018 13:05
Last Modified:18 Apr 2018 11:49
Publisher:Optical Society of America
ISSN:1094-4087
Funders:European Research Council (ERC) Advanced Investigator Grant (DYNALLO), Swiss National Science Foundation through the National Center of Competence and Research (NCCR) MUST
OA Status:Green
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:https://doi.org/10.1364/OE.25.002928
Project Information:
  • : Funder
  • : Grant ID
  • : Project TitleEuropean Research Council (ERC) Advanced Investigator Grant (DYNALLO)
  • : FunderSNSF
  • : Grant ID
  • : Project TitleSwiss National Science Foundation through the National Center of Competence and Research (NCCR) MUST

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