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Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport
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Marcus, Max, Knee, George C. and Datta, Animesh (2020) Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport. Faraday Discussions, 221 . pp. 110-132. doi:10.1039/c9fd00068b ISSN 0301-7249.
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Official URL: https://doi.org/10.1039/c9fd00068b
Abstract
The role of quantum effects in excitonic energy transport (EET) has been scrutinised intensely and with increasingly sophisticated experimental techniques. This increased complexity requires invoking correspondingly elaborate models to fit spectroscopic data before molecular parameters can be extracted. Possible quantum effects in EET can then be studied, but the conclusions are strongly contingent on the efficacy of the fitting and the accuracy of the model. To circumvent this challenge, we propose a witness for quantum coherence in EET that can be extracted directly from two-pulse pump–probe spectroscopy experimental data. We provide simulations to judge the feasibility of our approach. Somewhat counterintuitively, our protocol does not probe quantum coherence directly, but only indirectly through its implicit deletion. It allows for classical models with no quantum coherence to be decisively ruled out.
Item Type: | Journal Article | |||||||||
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Subjects: | Q Science > QC Physics Q Science > QD Chemistry |
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics | |||||||||
Library of Congress Subject Headings (LCSH): | Quantum field theory, Phase transformations (Statistical physics) , Energy transfer , Two-dimensional electronic-vibrational spectroscopy | |||||||||
Journal or Publication Title: | Faraday Discussions | |||||||||
Publisher: | Royal Society of Chemistry | |||||||||
ISSN: | 0301-7249 | |||||||||
Official Date: | 1 January 2020 | |||||||||
Dates: |
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Volume: | 221 | |||||||||
Page Range: | pp. 110-132 | |||||||||
DOI: | 10.1039/c9fd00068b | |||||||||
Status: | Peer Reviewed | |||||||||
Publication Status: | Published | |||||||||
Access rights to Published version: | Restricted or Subscription Access | |||||||||
Date of first compliant deposit: | 21 October 2019 | |||||||||
Date of first compliant Open Access: | 21 October 2019 | |||||||||
RIOXX Funder/Project Grant: |
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