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Titolo:
Time-resolved fluorescence of polarizable chromophores
Autore:
Matyushov, DV;
Indirizzi:
Arizona State Univ, Dept Chem & Biochem, Tempe, AZ 85287 USA Arizona StateUniv Tempe AZ USA 85287 Chem & Biochem, Tempe, AZ 85287 USA
Titolo Testata:
JOURNAL OF CHEMICAL PHYSICS
fascicolo: 19, volume: 115, anno: 2001,
pagine: 8933 - 8941
SICI:
0021-9606(20011115)115:19<8933:TFOPC>2.0.ZU;2-C
Fonte:
ISI
Lingua:
ENG
Soggetto:
ELECTRON-TRANSFER REACTIONS; POLAR SOLVATION DYNAMICS; STOKES SHIFT; NONEQUILIBRIUM SOLVATION; DEPENDENT FLUORESCENCE; COMPUTER-SIMULATION; DIELECTRIC FRICTION; LINE-SHAPES; COUMARIN-153; SOLVENT;
Tipo documento:
Article
Natura:
Periodico
Settore Disciplinare:
Physical, Chemical & Earth Sciences
Citazioni:
47
Recensione:
Indirizzi per estratti:
Indirizzo: Matyushov, DV Arizona State Univ, Dept Chem & Biochem, Tempe, AZ 85287 USAArizona State Univ Tempe AZ USA 85287 , Tempe, AZ 85287 USA
Citazione:
D.V. Matyushov, "Time-resolved fluorescence of polarizable chromophores", J CHEM PHYS, 115(19), 2001, pp. 8933-8941

Abstract

The paper reports an exact solution for spectral profiles of time-resolvedfluorescence following a broad-band excitation producing changes in both the chromophore's dipole moment and the polarizability. The problem is formulated in terms of a two-state chromophore with a bilinear coupling to a Gaussian solvent mode. Closed-form solutions for the time-dependent spectral shift and width are obtained. These two transient spectral moments are sufficient to generate transient, non-Gaussian band-shapes by using the proposedformalism. An approximately linear relation between the normalized shift and width time correlation functions is found. The Stokes shift correlation function is virtually insensitive to the nonlinear solute-solvent effects, in spite of dramatic transient changes in the spectral width. Depending on chromophore's parameters, the transient line shape can be well approximatedby a nonstationary Gaussian process or shows clearly non-Gaussian statistics. The model is extended to treat heterogeneous solvent dynamics. (C) 2001American Institute of Physics.

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Documento generato il 27/05/20 alle ore 13:47:51