2015
DOI: 10.1103/physrevlett.114.026402
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Dynamics of the Excitonic Coupling in Organic Crystals

Abstract: We show that the excitonic coupling in molecular crystals undergoes very large fluctuation at room temperature as a result of the combined thermal motions of the nuclei. This observation dramatically affects the description of exciton transport in organic crystals and any other phenomenon (like singlet fission or exciton dissociation) that originates from an exciton in a molecular crystal or thin-film. This unexpected result is due to the predominance of the shortrange excitonic coupling mechanisms (exchange, … Show more

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Cited by 128 publications
(193 citation statements)
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“…The regime of exciton transport (coherent or incoherent) is determined by the relative strength of the excitonic coupling and the exciton-phonon coupling. [35][36][37] Furthermore, short range interactions at finite temperature cause strong fluctuations in the excitonic coupling 3,13,36 which in some instances can influence or limit the energy transfer dynamics. [37][38][39] In photosynthesis, light absorption and efficient transport of the excitation energy is achieved by clusters of chromophores in proteins commonly called light harvesting complexes (LHCs).…”
Section:   a B A Bmentioning
confidence: 99%
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“…The regime of exciton transport (coherent or incoherent) is determined by the relative strength of the excitonic coupling and the exciton-phonon coupling. [35][36][37] Furthermore, short range interactions at finite temperature cause strong fluctuations in the excitonic coupling 3,13,36 which in some instances can influence or limit the energy transfer dynamics. [37][38][39] In photosynthesis, light absorption and efficient transport of the excitation energy is achieved by clusters of chromophores in proteins commonly called light harvesting complexes (LHCs).…”
Section:   a B A Bmentioning
confidence: 99%
“…3,4 For the study of the quantum mechanical evolution of excited states it has become commonplace to evaluate the excitonic coupling for a large number of structures, e.g. those deriving from a molecular dynamics simulation [5][6][7][8][9][10][11][12][13] or representing the interaction between chromophores in an amorphous system. [14][15][16][17][18][19][20] To perform these large scale simulations efficiently, to rationalize the observed properties and to design new materials it is important to identify the main components of the excitonic coupling and assess their relative importance.…”
Section: Introductionmentioning
confidence: 99%
“…16,18 A few examples in related self-assembled systems (porphyrins) have shown that exciton diffusion can efficiently occur by means of a coherent mechanism. 19 Recently, an octa(butyl)-substituted metal-free phthalocyanine, H2-OBPc (1,4,8,11,15,18,22,25-octabutoxy-29H,31H-phthalocyanine, see Figure 1a) has been synthesized and exhibited good crystallinity properties (1D π-stacked arrangements, see Figure 1b) in thin films. 20,21 The high degree of crystallinity of the solution-processed thin films allowed Rawat et al to investigate the correlation between long-range order and the nature of the lowest exciton states of the aggregate.…”
Section: Introductionmentioning
confidence: 99%
“…22,23 Regardless of the exciton diffusion mechanism invoked, the transport of molecular excitons is mainly governed by the excitonic coupling (J) between the excited states localized on the molecular units (Frenkel excited states). 5,24 In Pc systems, the two lowestenergy singlet excited states (commonly known as Q-bands 25 ) are almost degenerate in energy and, thus, both excited states may participate in the exciton transport of Pc molecular crystals or aggregates.…”
Section: Introductionmentioning
confidence: 99%
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