DC Field | Value | Language |
---|---|---|
dc.contributor.author | Hsieh, CC | - |
dc.contributor.author | Chou, PT | - |
dc.contributor.author | Shih, CW | - |
dc.contributor.author | Chuang, WT | - |
dc.contributor.author | Chung, MW | - |
dc.contributor.author | Lee, J | - |
dc.contributor.author | Joo, T | - |
dc.date.accessioned | 2016-03-31T09:44:41Z | - |
dc.date.available | 2016-03-31T09:44:41Z | - |
dc.date.created | 2011-05-16 | - |
dc.date.issued | 2011-03-09 | - |
dc.identifier.issn | 0002-7863 | - |
dc.identifier.other | 2011-OAK-0000023461 | - |
dc.identifier.uri | https://oasis.postech.ac.kr/handle/2014.oak/17526 | - |
dc.description.abstract | Initiated by excited-state intramolecular proton transfer (ESIPT) reaction, an overall reaction cycle of 4-(2-hydroxybenzylidene)-1,2-dimethyl-1H-imidazol-5(4H)-one (o-HBDI), an analogue of the core chromophore of the green fluorescent protein (GFP), has been investigated. In contrast to the native GFP core, 4-(4-hydroxybenzylidene)-1,2-dimethyl-1H-imidazol-5(411)-one (p-HBDI), which requires hydrogen-bonding relay to accomplish proton transfer in vivo, o-HBDI possesses a seven-membered-ring intramolecular hydrogen bond and thus provides an ideal system for mimicking an intrinsic proton-transfer reaction. Upon excitation, ESIPT takes place in o-HBDI, resulting in a similar to 600 nm proton-transfer tautomer emission. The o-HBDI tautomer emission, resolved by fluorescence upconversion, is comprised of an instantaneous rise to a few hundred femtosecond oscillation in the early relaxation stage. Frequency analysis derived from ultrashort pulse gives two low-frequency vibrations at 115 and 236 cm(-1), corresponding to skeletal deformation motions associated with the hydrogen bond. The results further conclude that ESIPT in o-HBDI is essentially triggered by low-frequency motions and maybe barrierless along the reaction coordinate. Femtosecond UV/vis transient absorption spectra also provide supplementary evidence for the structural evolution during the reaction. In CH3CN, an instant rise of a 530 nm transient is resolved, which then undergoes 7.8 Ps decay, accompanied by the growth of a rather long-lived 580 nm transient species. It is thus concluded that following ESIPT the cis-proton transfer isomer undergoes cis-trans-isomerization. The results of viscosity-dependent dynamics are in favor of the one-bond-flip mechanism, which is in contrast to the volume-conserving isomerization behavior for cis-stilbene and p-HBDI. Further confirmation is given by the picosecond femtosecond transient IR absorption spectra, where several new and long-lived IR bands in the range of 1400-1500 cm I are assigned to the phenyl in-plane breathing motions of the trans-proton transfer tautomer. Monitored by the nanosecond transient absorption, the 580 nm transient undergoes a similar to 7.7 mu s decay constant, accompanied by the growth of a new similar to 500 nm band. The latter is assigned to a deprotonated tautomer species, which then undergoes the ground-state reverse proton recombination to the original o-HBDI in similar to 50 mu s, achieving an overall, reversible proton transfer cycle. This assignment is unambiguously supported by pump probe laser induced fluorescence studies. On these standpoints, a comparison of photophysical properties among o-HBDI, p-HBDI, and wild-type GFP is discussed in detail. | - |
dc.description.statementofresponsibility | X | - |
dc.language | English | - |
dc.publisher | AMER CHEMICAL SOC | - |
dc.relation.isPartOf | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | - |
dc.subject | EXCITED-STATE DYNAMICS | - |
dc.subject | ULTRAFAST VIBRATIONAL SPECTROSCOPY | - |
dc.subject | MOLECULAR-ORBITAL THEORY | - |
dc.subject | CHARGE-TRANSFER REACTION | - |
dc.subject | CIS-STILBENE | - |
dc.subject | TEMPERATURE-DEPENDENCE | - |
dc.subject | FEMTOSECOND DYNAMICS | - |
dc.subject | VARIANT S65T/H148D | - |
dc.subject | GFP | - |
dc.subject | PHOTOISOMERIZATION | - |
dc.title | Comprehensive Studies on an Overall Proton Transfer Cycle of the ortho-Green Fluorescent Protein Chromophore | - |
dc.type | Article | - |
dc.contributor.college | 화학과 | - |
dc.identifier.doi | 10.1021/JA107945M | - |
dc.author.google | Hsieh, CC | - |
dc.author.google | Chou, PT | - |
dc.author.google | Shih, CW | - |
dc.author.google | Chuang, WT | - |
dc.author.google | Chung, MW | - |
dc.author.google | Lee, J | - |
dc.author.google | Joo, T | - |
dc.relation.volume | 133 | - |
dc.relation.issue | 9 | - |
dc.relation.startpage | 2932 | - |
dc.relation.lastpage | 2943 | - |
dc.contributor.id | 10092693 | - |
dc.relation.journal | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | - |
dc.relation.index | SCI급, SCOPUS 등재논문 | - |
dc.relation.sci | SCI | - |
dc.collections.name | Journal Papers | - |
dc.type.rims | ART | - |
dc.identifier.bibliographicCitation | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.133, no.9, pp.2932 - 2943 | - |
dc.identifier.wosid | 000289455200030 | - |
dc.date.tcdate | 2019-01-01 | - |
dc.citation.endPage | 2943 | - |
dc.citation.number | 9 | - |
dc.citation.startPage | 2932 | - |
dc.citation.title | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | - |
dc.citation.volume | 133 | - |
dc.contributor.affiliatedAuthor | Joo, T | - |
dc.identifier.scopusid | 2-s2.0-79952261486 | - |
dc.description.journalClass | 1 | - |
dc.description.journalClass | 1 | - |
dc.description.wostc | 90 | - |
dc.description.scptc | 81 | * |
dc.date.scptcdate | 2018-05-121 | * |
dc.type.docType | Article | - |
dc.subject.keywordPlus | EXCITED-STATE DYNAMICS | - |
dc.subject.keywordPlus | CIS-STILBENE | - |
dc.subject.keywordPlus | TEMPERATURE-DEPENDENCE | - |
dc.subject.keywordPlus | FEMTOSECOND DYNAMICS | - |
dc.subject.keywordPlus | VARIANT S65T/H148D | - |
dc.subject.keywordPlus | PHOTOISOMERIZATION | - |
dc.subject.keywordPlus | ISOMERIZATION | - |
dc.subject.keywordPlus | SPECTROSCOPY | - |
dc.subject.keywordPlus | ABSORPTION | - |
dc.subject.keywordPlus | ENERGY | - |
dc.relation.journalWebOfScienceCategory | Chemistry, Multidisciplinary | - |
dc.description.journalRegisteredClass | scie | - |
dc.description.journalRegisteredClass | scopus | - |
dc.relation.journalResearchArea | Chemistry | - |
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