Modeling of ultrafast time-resolved fluorescence applied to a weakly coupled chromophore pair

被引：8

作者：

Balevicius, V., Jr. ^{[1
]}

Valkunas, L. ^{[1
,2
]}

Abramavicius, D. ^{[1
]}

机构：

[1] Vilnius State Univ, Fac Phys, Dept Theoret Phys, LT-10222 Vilnius, Lithuania

[2] Ctr Phys Sci & Technol, Inst Phys, LT-02300 Vilnius, Lithuania

来源：

JOURNAL OF CHEMICAL PHYSICS | 2015年 / 143卷 / 07期

关键词：

LH2; BACTERIOCHLOROPHYLL; SPONTANEOUS EMISSION; EXCITED-STATES; COHERENCE; DYNAMICS; SPECTROSCOPY; POLARONS; SPECTRA;

D O I：

10.1063/1.4928281

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

We present theory for calculating the third-order non-linear response function of a molecular aggregate in the weak inter-chromophore coupling regime. This approach is based on the perturbative expansion of the system evolution with respect to the resonance coupling, while the system-bath interaction is treated non-perturbatively by means of cumulant expansion. An explicit expression for the time-resolved fluorescence signal is then obtained. This allows us to investigate the ultrafast time-dependent Stokes shift, signatures of coherent dynamics, and the excitonic polaron formation in the excited state of the aggregate. Numerical simulations of the time-resolved fluorescence spectra of a pair of coupled molecules demonstrate these effects. (C) 2015 AIP Publishing LLC.

引用

页数：10

共 43 条

[31]

Mukamel S., 1995, Principles of nonlinear optical spectroscopy

[32] Coherent oscillations in ultrafast fluorescence of photoactive yellow protein [J].

Nakamura, Ryosuke ;

Hamada, Norio ;

Ichida, Hideki ;

Tokunaga, Fumio ;

Kanematsu, Yasuo .

JOURNAL OF CHEMICAL PHYSICS, 2007, 127 (21)

[33] DNA/RNA nucleotides and nucleosides: direct measurement of excited-state lifetimes by femtosecond fluorescence up-conversion [J].

Peon, J ;

Zewail, AH .

CHEMICAL PHYSICS LETTERS, 2001, 348 (3-4) :255-262

[34] Two-dimensional optical three-pulse photon echo spectroscopy.: II.: Signatures of coherent electronic motion and exciton population transfer in dimer two-dimensional spectra [J].

Pisliakov, Andrei V. ;

Mancal, Tomas ;

Fleming, Graham R. .

JOURNAL OF CHEMICAL PHYSICS, 2006, 124 (23)

[35] Combined treatment of relaxation and fluctuation dynamics in the calculation of two-dimensional electronic spectra [J].

Seibt, Joachim ;

Pullerits, Tonu .

JOURNAL OF CHEMICAL PHYSICS, 2014, 141 (11)

[36] Mapping the Evolution of Spatial Exciton Coherence through Time-Resolved Fluorescence [J].

Tempelaar, Roel ;

Spano, Frank C. ;

Knoester, Jasper ;

Jansen, Thomas L. C. .

JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2014, 5 (09) :1505-1510

[37] A disordered polaron model for polarized fluorescence excitation spectra of LH1 and LH2 bacteriochlorophyll antenna aggregates [J].

Trinkunas, G ;

Freiberg, A .

JOURNAL OF LUMINESCENCE, 2006, 119 :105-110

[38] SHORT-TIME FLUORESCENCE STOKES SHIFT DYNAMICS [J].

Ungar, Lowell W. ;

Cina, Jeffrey A. .

ADVANCES IN CHEMICAL PHYSICS <D>, 1997, 100 :171-228

[39]

Valkunas L., 2013, MOL EXCITATION DYNAM

[40]

Van Amerongen H., 2000, Photosynthetic Excitons

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