Non-Markovian effects in time-resolved fluorescence spectrum of molecular aggregates: Tracing polaron formation

被引：46

作者：

Gelzinis, Andrius ^{[1
,2
]}

Abramavicius, Darius ^{[1
,3
]}

Valkunas, Leonas ^{[1
,2
]}

机构：

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

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

[3] Jilin Univ, State Key Lab Supramol Complexes, Changchun 130012, Peoples R China

来源：

PHYSICAL REVIEW B | 2011年 / 84卷 / 24期

关键词：

QUANTUM COHERENCE; OPTICAL-SPECTRA; ENERGY-TRANSFER; DYNAMICS; PHOTOSYNTHESIS; SYSTEM; SPECTROSCOPY; SIMULATION; TRANSPORT; EXCITONS;

D O I：

10.1103/PhysRevB.84.245430

中图分类号：

T [工业技术];

学科分类号：

08 ;

摘要：

Time-resolved fluorescence spectroscopy of molecular aggregates is described using the response function theory, which incorporates exciton dynamics through nonequilibrium Green's functions. The dynamics are simulated using nonperturbative density matrix theory, which allows us to describe spectral and temporal signatures of various system-bath coupling regimes. We find that the conventional excitonic picture of eigenstates is valid in the Markovian regime. In the non-Markovian regime, the exciton concept breaks down and renormalized quantities can be introduced. Effective intermolecular coupling, widely used in polaron theories, can be used to account for the effects of the bath.

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页数：14

相关论文

共 56 条

[31] Polarons, localization, and excitonic coherence in superradiance of biological antenna complexes [J].

Meier, T ;

Zhao, Y ;

Chernyak, V ;

Mukamel, S .

JOURNAL OF CHEMICAL PHYSICS, 1997, 107 (10) :3876-3893

[32]

Mukamel S., 1995, Principles of Nonlinear Optical Spectroscopy

[33] 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)

[34] Pathways and timescales of primary charge separation in the photosystem II reaction center as revealed by a simultaneous fit of time-resolved fluorescence and transient absorption [J].

Novoderezhkin, VI ;

Andrizhiyevskaya, EG ;

Dekker, JP ;

van Grondelle, R .

BIOPHYSICAL JOURNAL, 2005, 89 (03) :1464-1481

[35] Theory and Simulation of the Environmental Effects on FMO Electronic Transitions [J].

Olbrich, Carsten ;

Struempfer, Johan ;

Schulten, Klaus ;

Kleinekathoefer, Ulrich .

JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2011, 2 (14) :1771-1776

[36] Electronic coherence dephasing in excitonic molecular complexes: Role of Markov and secular approximations [J].

Olsina, Jan ;

Mancal, Tomas .

JOURNAL OF MOLECULAR MODELING, 2010, 16 (11) :1765-1778

[37] Davydov Splitting of Excitons in Cyclic Bacteriochlorophyll a Nanoaggregates of Bacterial Light-Harvesting Complexes between 4.5 and 263 K [J].

Pajusalu, Mihkel ;

Raetsep, Margus ;

Trinkunas, Gediminas ;

Freiberg, Arvi .

CHEMPHYSCHEM, 2011, 12 (03) :634-644

[38] Theory of optical spectra of photosystem II reaction centers: Location of the triplet state and the identity of the primary electron donor [J].

Raszewski, G ;

Saenger, W ;

Renger, T .

BIOPHYSICAL JOURNAL, 2005, 88 (02) :986-998

[39]

Renger T, 2001, PHYS REP, V343, P138, DOI 10.1016/S0370-1573(00)00078-8

[40] Two-dimensional electronic spectroscopy and photosynthesis: Fundamentals and applications to photosynthetic light-harvesting [J].

Schlau-Cohen, Gabriela S. ;

Ishizaki, Akihito ;

Fleming, Graham R. .

CHEMICAL PHYSICS, 2011, 386 (1-3) :1-22

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