Chiroptical nature of two-exciton states of light-harvesting complex: Doubly resonant three-wave-mixing spectroscopy
DC Field | Value | Language |
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dc.contributor.author | Lee, Hochan | - |
dc.contributor.author | Cheon, Sangheon | - |
dc.contributor.author | Cho, Minhaeng | - |
dc.date.accessioned | 2021-09-08T02:22:15Z | - |
dc.date.available | 2021-09-08T02:22:15Z | - |
dc.date.created | 2021-06-11 | - |
dc.date.issued | 2010-06-14 | - |
dc.identifier.issn | 0021-9606 | - |
dc.identifier.uri | https://scholar.korea.ac.kr/handle/2021.sw.korea/116242 | - |
dc.description.abstract | Photosynthetic light-harvesting complex is a coupled multichromophore system. Due to electronic couplings between neighboring chlorophylls in the complex, the one- and two-exciton states are delocalized and they can be written as linear combinations of singly and doubly excited configurations, respectively. Despite that the chiroptical properties of one-exciton states in such a multichromophore system have been investigated by using linear optical activity measurement techniques; those of two-exciton states have not been studied before due to a lack of appropriate measurement methods. Here, we present a theoretical description on chiroptical chi((2)) spectroscopy and show that it can be used to investigate such properties of a photosynthetic light-harvesting system, which is the Fenna-Matthews-Olson complex, consisting of seven bacteriochlorophylls in its protein subunit. To simulate the doubly resonant sum- and difference-frequency-generation spectra of the complex, one- and two-exciton transition dipoles were calculated. Carrying out quantum chemistry calculations of electronically excited states of a model bacteriochlorophyll system and taking into account the dipole-induced dipole electronic transition processes between the ground state and two-exciton states, we could calculate the two-dimensional sum-frequency-generation spectra revealing dominant second-order chiroptical transition pathways and involved one- and two-exciton states. It is believed that the present computational scheme and the theoretically proposed doubly resonant two-dimensional three-wave-mixing spectroscopy would be of use to shed light on the chiroptical natures of two-exciton states of arbitrary coupled multichromophore systems. (C) 2010 American Institute of Physics. [doi:10.1063/1.3432624] | - |
dc.language | English | - |
dc.language.iso | en | - |
dc.publisher | AMER INST PHYSICS | - |
dc.subject | EXCITATION-ENERGY TRANSFER | - |
dc.subject | EXCITON INTERACTION | - |
dc.subject | FMO COMPLEX | - |
dc.subject | BACTERIOCHLOROPHYLL | - |
dc.subject | PROTEIN | - |
dc.subject | DYNAMICS | - |
dc.title | Chiroptical nature of two-exciton states of light-harvesting complex: Doubly resonant three-wave-mixing spectroscopy | - |
dc.type | Article | - |
dc.contributor.affiliatedAuthor | Lee, Hochan | - |
dc.contributor.affiliatedAuthor | Cho, Minhaeng | - |
dc.identifier.doi | 10.1063/1.3432624 | - |
dc.identifier.scopusid | 2-s2.0-77953548905 | - |
dc.identifier.wosid | 000278858400042 | - |
dc.identifier.bibliographicCitation | JOURNAL OF CHEMICAL PHYSICS, v.132, no.22 | - |
dc.relation.isPartOf | JOURNAL OF CHEMICAL PHYSICS | - |
dc.citation.title | JOURNAL OF CHEMICAL PHYSICS | - |
dc.citation.volume | 132 | - |
dc.citation.number | 22 | - |
dc.type.rims | ART | - |
dc.type.docType | Article | - |
dc.description.journalClass | 1 | - |
dc.description.journalRegisteredClass | scie | - |
dc.description.journalRegisteredClass | scopus | - |
dc.relation.journalResearchArea | Chemistry | - |
dc.relation.journalResearchArea | Physics | - |
dc.relation.journalWebOfScienceCategory | Chemistry, Physical | - |
dc.relation.journalWebOfScienceCategory | Physics, Atomic, Molecular & Chemical | - |
dc.subject.keywordPlus | EXCITATION-ENERGY TRANSFER | - |
dc.subject.keywordPlus | EXCITON INTERACTION | - |
dc.subject.keywordPlus | FMO COMPLEX | - |
dc.subject.keywordPlus | BACTERIOCHLOROPHYLL | - |
dc.subject.keywordPlus | PROTEIN | - |
dc.subject.keywordPlus | DYNAMICS | - |
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