Monte Carlo wavefunction approach to the exciton dynamics of molecular aggregates with exciton–phonon coupling

Ohta, Suguru; Nakano, Masayoshi; Kishi, Ryohei; Takahashi, Hideaki; Furukawa, Shunsuke

doi:10.1016/j.cplett.2005.11.052

Cited by 8 publications

(5 citation statements)

References 20 publications

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“…The MCWF method was originally developed for dissipative processes in quantum optics [58]. The main advantage of MCWF is the fact that one only needs to simulate the wave function rather than the density operator [59]. Our approach can potentially be used to enhance energy transfer efficiency via engineering quantum interference effects.…”

Section: Discussionmentioning

confidence: 99%

Environment-assisted quantum walks in photosynthetic energy transfer

Mohseni

Rebentrost

Lloyd

et al. 2008

The Journal of Chemical Physics

1,167

1,439

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Underlying physical principles for the high efficiency of excitation energy transfer in light-harvesting complexes are not fully understood. Notably, the degree of robustness of these systems for transporting energy is not known considering their realistic interactions with vibrational and radiative environments within the surrounding solvent and scaffold proteins. In this work, we employ an efficient technique to estimate energy transfer efficiency of such complex excitonic systems. We observe that the dynamics of the Fenna-Matthews-Olson (FMO) complex leads to optimal and robust energy transport due to a convergence of energy scales among all important internal and external parameters. In particular, we show that the FMO energy transfer efficiency is optimum and stable with respect to important parameters of environmental interactions including reorganization energy λ, bath frequency cutoff γ , temperature T, and bath spatial correlations. We identify the ratio of k B λT /¯γ g as a single key parameter governing quantum transport efficiency, where g is the average excitonic energy gap. © 2014 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License. [http://dx.

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Section: Discussionmentioning

confidence: 99%

Environment-assisted quantum walks in photosynthetic energy transfer

Mohseni

Rebentrost

Lloyd

et al. 2008

The Journal of Chemical Physics

1,167

1,439

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“…The quantum dynamics of excitons can be numerically simulated using various methods, including density matrix evolution schemes [57,58] and also diffusion [59,60] and quantum jump [61,62] wavefunction approaches. The latter are based on propagating the system's wavefunction rather than the density matrix and are therefore computationally more convenient to be employed for modeling large systems.…”

Section: A Hamiltonian and Single Exciton Dynamicsmentioning

confidence: 99%

Exciton transport in thin-film cyanine dye J-aggregates

Valleau

Saikin

Yung

et al. 2012

The Journal of Chemical Physics

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We present a theoretical model for the study of exciton dynamics in J-aggregated monolayers of fluorescent dyes. The excitonic evolution is described by a Monte-Carlo wave function approach which allows for a unified description of the quantum (ballistic) and classical (diffusive) propagation of an exciton on a lattice in different parameter regimes. The transition between the ballistic and diffusive regime is controlled by static and dynamic disorder. As an example, the model is applied to three cyanine dye J-aggregates: TC, TDBC, and U3. Each of the molecule-specific structure and excitation parameters are estimated using time-dependent density functional theory. The exciton diffusion coefficients are calculated and analyzed for different degrees of film disorder and are correlated to the physical properties and the structural arrangement of molecules in the aggregates. Further, exciton transport is anisotropic and dependent on the initial exciton energy. The upper-bound estimation of the exciton diffusion length in the TDBC thin-film J-aggregate is of the order of hundreds of nanometers, which is in good qualitative agreement with the diffusion length estimated from experiments.

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“…These allow for the efficient description of the interaction between excitons and nuclear vibrations, i.e., phonons, and account for both coherent and incoherent dynamics. Quantum master equations have therefore been applied to a variety of exciton transport problems in OSCs, such as natural photosynthetic complexes [35][36][37][38], molecular aggregates [39][40][41][42], and disordered systems [34,43]. A key insight from this body of literature is that exciton-phonon interactions have an essential role for exciton transport in OSCs.…”

Section: Introductionmentioning

confidence: 99%

Exciton transport in amorphous polymers and the role of morphology and thermalisation

Campaioli,

Cole

2021

Preprint

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Understanding the transport mechanism of electronic excitations in conjugated polymers is key to advancing organic optoelectronic applications, such as solar cells, OLEDs and flexible electronics. While crystalline polymers can be studied using solid-state techniques based on lattice periodicity, the characterisation of amorphous polymers is hindered by an intermediate regime of disorder and the associated lack of symmetries. To overcome these hurdles we use a reduced state quantum master equation approach based on the Merrifield exciton formalism. Using this model we study exciton transport in conjugated polymers and its dependence on morphology and temperature. Exciton dynamics consists of a thermalisation process, whose features depend on the relative strength of thermal energy, electronic couplings and disorder, resulting in remarkably different transport regimes. By applying this method to representative systems based on poly(p-phenylene vinylene) (PPV) we obtain insight into the role of temperature and disorder on localisation, charge separation, non-equilibrium dynamics, and experimental accessibility of thermal equilibrium states of excitons in amorphous polymers.

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Monte Carlo wavefunction approach to the exciton dynamics of molecular aggregates with exciton–phonon coupling

Cited by 8 publications

References 20 publications

Environment-assisted quantum walks in photosynthetic energy transfer

Environment-assisted quantum walks in photosynthetic energy transfer

Exciton transport in thin-film cyanine dye J-aggregates

Exciton transport in amorphous polymers and the role of morphology and thermalisation

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