Electric Field Keeps Chromophore Planar and Produces High Yield Fluorescence in Green Fluorescent Protein

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dc.contributor.authorPark, Jae Wooko
dc.contributor.authorRhee, Young Minko
dc.date.accessioned2017-08-16T08:54:10Z-
dc.date.available2017-08-16T08:54:10Z-
dc.date.created2017-08-07-
dc.date.created2017-08-07-
dc.date.issued2016-10-
dc.identifier.citationJOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.138, no.41, pp.13619 - 13629-
dc.identifier.issn0002-7863-
dc.identifier.urihttp://hdl.handle.net/10203/225356-
dc.description.abstractThe green fluorescent protein and its designed variants fluoresce efficiently. Because the isolated chromophore is not fluorescent in a practical sense, it is apparent that the protein environment plays a crucial role in its efficiency. Because of various obstacles in studying excited state dynamics of complex systems, however, the detailed mechanism of this efficiency enhancement is not yet clearly elucidated. Here, by adopting excited state nonadiabatic molecular dynamics simulations together with an interpolated quantum chemical potential model of the chromophore, we find that the strong electric field from the protein matrix contributes dominantly to the motional restriction of the chromophore. The delay in twisting motion subsequently obstructs the nonradiative decay that competes with fluorescence, leading naturally to an enhancement in light-emitting efficiency. Surprisingly, steric constraints make only a minor contribution to these aspects. Through residue specific analyses, we identify a group of key residues that control the excited state behavior. Testing a series of mutant GFPs with different brightnesses also supports the view regarding the importance of protein electrostatics. Our findings may provide a useful guide toward designing new fluorescent chemical systems in the future.-
dc.languageEnglish-
dc.publisherAMER CHEMICAL SOC-
dc.subjectPOTENTIAL-ENERGY SURFACES-
dc.subjectEXCITED-STATE DYNAMICS-
dc.subjectFAST INTERNAL-CONVERSION-
dc.subjectMOLECULAR-DYNAMICS-
dc.subjectGFP CHROMOPHORE-
dc.subjectPROTON-TRANSFER-
dc.subjectSHEPARD INTERPOLATION-
dc.subjectMECHANICS SIMULATIONS-
dc.subjectQUANTUM DECOHERENCE-
dc.subjectEMISSION-
dc.titleElectric Field Keeps Chromophore Planar and Produces High Yield Fluorescence in Green Fluorescent Protein-
dc.typeArticle-
dc.identifier.wosid000385992100031-
dc.identifier.scopusid2-s2.0-84992168879-
dc.type.rimsART-
dc.citation.volume138-
dc.citation.issue41-
dc.citation.beginningpage13619-
dc.citation.endingpage13629-
dc.citation.publicationnameJOURNAL OF THE AMERICAN CHEMICAL SOCIETY-
dc.identifier.doi10.1021/jacs.6b06833-
dc.contributor.localauthorRhee, Young Min-
dc.contributor.nonIdAuthorPark, Jae Woo-
dc.description.isOpenAccessN-
dc.type.journalArticleArticle-
dc.subject.keywordPlusPOTENTIAL-ENERGY SURFACES-
dc.subject.keywordPlusEXCITED-STATE DYNAMICS-
dc.subject.keywordPlusFAST INTERNAL-CONVERSION-
dc.subject.keywordPlusMOLECULAR-DYNAMICS-
dc.subject.keywordPlusGFP CHROMOPHORE-
dc.subject.keywordPlusPROTON-TRANSFER-
dc.subject.keywordPlusSHEPARD INTERPOLATION-
dc.subject.keywordPlusMECHANICS SIMULATIONS-
dc.subject.keywordPlusQUANTUM DECOHERENCE-
dc.subject.keywordPlusEMISSION-
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