Theoretical description of quantum effects in multi-chromophoric aggregates

Zimanyi, Eric N.; Silbey, R.

doi:10.1098/rsta.2011.0204

Cited by 50 publications

(55 citation statements)

References 64 publications

(111 reference statements)

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“…(24) with that from the time-convolutionless second-order polaron master equation without the secular and Markov approximations [55]. The results are plotted in Fig.…”

Section: Validity Of the Ptrementioning

confidence: 76%

Non-canonical distribution and non-equilibrium transport beyond weak system-bath coupling regime: A polaron transformation approach

Cao

2016

Front. Phys.

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The concept of polaron, emerged from condense matter physics, describes the dynamical interaction of moving particle with its surrounding bosonic modes. This concept has been developed into a useful method to treat open quantum systems with a complete range of system-bath coupling strength. Especially, the polaron transformation approach shows its validity in the intermediate coupling regime, in which the Redfield equation or Fermi's golden rule will fail. In the polaron frame, the equilibrium distribution carried out by perturbative expansion presents a deviation from the canonical distribution, which is beyond the usual weak coupling assumption in thermodynamics. A polaron transformed Redfield equation (PTRE) not only reproduces the dissipative quantum dynamics but also provides an accurate and efficient way to calculate the non-equilibrium steady states. Applications of the PTRE approach to problems such as exciton diffusion, heat transport and light-harvesting energy transfer are presented.

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“…(24) with that from the time-convolutionless second-order polaron master equation without the secular and Markov approximations [55]. The results are plotted in Fig.…”

Section: Validity Of the Ptrementioning

confidence: 76%

Non-canonical distribution and non-equilibrium transport beyond weak system-bath coupling regime: A polaron transformation approach

Cao

2016

Front. Phys.

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“…We compare the results from the above secular polaron master equation with that of the more accurate time-convolutionless second-order polaron master equation 37 without the secular and Markov approximations for an unbiased two-site system. The results are plotted in Figure 4.…”

Section: Discussionmentioning

confidence: 99%

Coherent quantum transport in disordered systems: A unified polaron treatment of hopping and band-like transport

Lee

Moix

Cao

2015

The Journal of Chemical Physics

103

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Quantum transport in disordered systems is studied using a polaron-based master equation. The polaron approach is capable of bridging the results from the coherent band-like transport regime governed by the Redfield equation to incoherent hopping transport in the classical regime. A non-monotonic dependence of the diffusion coefficient is observed both as a function of temperature and system-phonon coupling strength. In the band-like transport regime, the diffusion coefficient is shown to be linearly proportional to the system-phonon coupling strength and vanishes at zero coupling due to Anderson localization. In the opposite classical hopping regime, we correctly recover the dynamics described by the Fermi's Golden Rule and establish that the scaling of the diffusion coefficient depends on the phonon bath relaxation time. In both the hopping and band-like transport regimes, it is demonstrated that at low temperature, the zero-point fluctuations of the bath lead to non-zero transport rates and hence a finite diffusion constant. Application to rubrene and other organic semiconductor materials shows a good agreement with experimental mobility data. C 2015 AIP Publishing LLC. [http://dx

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“…In contrast, despite their attraction in terms of simplicity, intuitive physical insight and efficiency, standard (e.g., Redfield) master equations are often invalid in regimes relevant to molecular complexes due to their limitation to weak system-environment couplings. 53,54 Though procedures such as the polaron transformation can be used to broaden the range of validity of Redfield master equations, [55][56][57][58][59][60][61][62][63] again be restricted, for example, to situations in which the high-frequency environmental response dominates. 57,[64][65][66] Recently, a master equation approach based on the reaction coordinate (RC) model (see Fig.…”

Section: Introductionmentioning

confidence: 99%

Energy transfer in structured and unstructured environments: Master equations beyond the Born-Markov approximations

Iles-Smith

Dijkstra

Lambert

et al. 2016

The Journal of Chemical Physics

125

164

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Criteria for the accuracy of small polaron quantum master equation in simulating excitation energy transfer dynamics J. Chem. Phys. 139, 224112 (2013) (2014)], we go beyond the commonly used Born-Markov approximations to incorporate system-environment correlations and the resultant non-Markovian dynamical effects. We obtain energy transfer dynamics for both underdamped and overdamped oscillator environments that are in perfect agreement with the numerical hierarchical equations of motion over a wide range of parameters. Furthermore, we show that the Zusman equations, which may be obtained in a semiclassical limit of the reaction coordinate model, are often incapable of describing the correct dynamical behaviour. This demonstrates the necessity of properly accounting for quantum correlations generated between the system and its environment when the Born-Markov approximations no longer hold. Finally, we apply the reaction coordinate formalism to the case of a structured environment comprising of both underdamped (i.e., sharply peaked) and overdamped (broad) components simultaneously. We find that though an enhancement of the dimer energy transfer rate can be obtained when compared to an unstructured environment, its magnitude is rather sensitive to both the dimer-peak resonance conditions and the relative strengths of the underdamped and overdamped contributions. C 2016 AIP Publishing LLC. [http://dx

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Theoretical description of quantum effects in multi-chromophoric aggregates

Cited by 50 publications

References 64 publications

Non-canonical distribution and non-equilibrium transport beyond weak system-bath coupling regime: A polaron transformation approach

Non-canonical distribution and non-equilibrium transport beyond weak system-bath coupling regime: A polaron transformation approach

Coherent quantum transport in disordered systems: A unified polaron treatment of hopping and band-like transport

Energy transfer in structured and unstructured environments: Master equations beyond the Born-Markov approximations

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