Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport
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 extrac...
| Main Authors: | , , |
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| Format: | Journal article |
| Language: | English |
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Royal Society of Chemistry
2019
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| _version_ | 1797095774751817728 |
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| author | Marcus, M Knee, GC Datta, A |
| author_facet | Marcus, M Knee, GC Datta, A |
| author_sort | Marcus, M |
| collection | OXFORD |
| description | 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. |
| first_indexed | 2024-03-07T04:32:44Z |
| format | Journal article |
| id | oxford-uuid:cee14cda-f8f9-477f-8445-d0df46ec2f2c |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-07T04:32:44Z |
| publishDate | 2019 |
| publisher | Royal Society of Chemistry |
| record_format | dspace |
| spelling | oxford-uuid:cee14cda-f8f9-477f-8445-d0df46ec2f2c2022-03-27T07:38:35ZTowards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transportJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:cee14cda-f8f9-477f-8445-d0df46ec2f2cEnglishSymplectic ElementsRoyal Society of Chemistry2019Marcus, MKnee, GCDatta, AThe 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. |
| spellingShingle | Marcus, M Knee, GC Datta, A Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport |
| title | Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport |
| title_full | Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport |
| title_fullStr | Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport |
| title_full_unstemmed | Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport |
| title_short | Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport |
| title_sort | towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport |
| work_keys_str_mv | AT marcusm towardsaspectroscopicprotocolforunambiguousdetectionofquantumcoherenceinexcitonicenergytransport AT kneegc towardsaspectroscopicprotocolforunambiguousdetectionofquantumcoherenceinexcitonicenergytransport AT dattaa towardsaspectroscopicprotocolforunambiguousdetectionofquantumcoherenceinexcitonicenergytransport |