Delocalization and Quantum Entanglement in Physical Systems

Dutta, Rajesh; Bagchi, Biman

doi:10.1021/acs.jpclett.9b00382

Cited by 7 publications

(14 citation statements)

References 39 publications

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“…We have used the temperature-independent QSLE to study efficient energy transfer dynamics. In our earlier studies, we have shown that the effect of temperature is pronounced in the intermediate coupling regime and explain its effect on the energy relaxation and equilibrium population − in the absence of trapping and radiative decay. We also have observed earlier that the inclusion of temperature slows down the excitation energy relaxation dynamics.…”

Section: Discussionmentioning

confidence: 81%

“…This is a nonperturbative method. We have discussed and employed this approach in our previous studies. − ,, We consider that fluctuations around each chromophore are spatially uncorrelated. That is, the fluctuating elements in the Hamiltonian at each chromophore site are independent of each other.…”

Section: Qsle Approachmentioning

confidence: 99%

“…In the presence of spatial and temporal correlations, this is a formidable task for a quantum system. Although the memory effects have been considered in describing excitation energy transfer dynamics using the hierarchical equation of motion (HEOM), − generalized Bloch Redfield equation, and temperature-corrected stochastic Liouville equation (SLE), − surprisingly very few of the descriptions are used to explore the optimal energy transfer in the presence of both radiative and nonradiative decay in different coupling regimes. Also, the important question of relationship with the classical rate description and its validity over different coupling regimes is explored here for the first time.…”

Section: Introductionmentioning

confidence: 99%

“…In our earlier studies, we explored the role of quantum coherence in the energy transfer processes in photosynthetic FMO complexes, , exciton diffusion, and line shape in a linear and cyclic model system. We also established a connection between steady-state quantum coherence and noncanonical population distribution in noisy environments for model and real open quantum systems .…”

Section: Introductionmentioning

confidence: 99%

“…The quantum coherence and interference effects were quantified in our earlier studies of energy transfer dynamics in photosynthetic systems in Markovian and non-Markovian limits. − Finite values of coherences were observed in both the Markovian and non-Markovian limit. However, the decay was faster for the Markovian limit than that of the non-Markovian limit.…”

Section: Introductionmentioning

confidence: 99%

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Excitation Energy Transfer Efficiency in Fluctuating Environments: Role of Quantum Coherence in the Presence of Memory Effects

Dutta

Bagchi

2021

J. Phys. Chem. A

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Several recent studies have interrogated the role of quantum coherence in affecting the transfer efficiency of an optical excitation to the designated "trap" state where the energy can be used for subsequent reactions, as in photosynthesis. However, these studies invoke a Markovian approximation for the time correlation function describing the environment-induced stochastic fluctuations. Here, we employ Kubo's quantum stochastic Liouville equation (QSLE) to include memory effects. We extend the existing QSLE scheme to introduce decay of a newly created excitation due to radiative and nonradiative channels and also by desired trapping toward the targeted chromophore. We show that the theoretical formalism based on the QSLE correctly reproduces the rate equation description in the Markovian limit, with the rate constants determined by an appropriate quantum limiting procedure. We find that under certain conditions, the efficiency of excitation transfer to the trap gains from the combined presence of quantum coherence and temporally correlated stochastic fluctuations. We work out different limiting situations in order to discover and quantify the optimum conditions for the energy transfer to the trapped state. We find that maximum energy transfer efficiency is achieved in the intermediate limit between coherent and incoherent transport.

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Section: Discussionmentioning

confidence: 81%

Section: Qsle Approachmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Excitation Energy Transfer Efficiency in Fluctuating Environments: Role of Quantum Coherence in the Presence of Memory Effects

Dutta

Bagchi

2021

J. Phys. Chem. A

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Importance of Intermonomer Couplings of the FMO Complex in Coherently Initiated Dynamics

Singh

Dasgupta

2020

J. Phys. Chem. B

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In this work, the hierarchical equation of motion approach was employed to study the excitation transfer efficiency (ETE) from the Fenna-Matthews-Olson (FMO) complex to the reaction center core complex (RCC). Further, the realistic initial pure state (created by the interaction of femtosecond laser pulse with the isolated FMO complex) was used in the presence of an inhomogeneous protein environment. We observed the same amount of excitation transfer from the FMO to the RCC, in agreement with the experiment using femtosecond absorption spectroscopy. Simulation analysis shows weak intermonomer couplings are strongly affecting the dynamics of ETE, which implies that all the monomers of the FMO complex need to be considered as connected with the RCC pigment for a better estimate of the ETE.

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Quantum Coherence and Its Signatures in Extended Quantum Systems

Dutta

Bagchi

2020

J. Phys. Chem. B

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Quantum coherence controls almost every aspect of static and dynamic response of a strongly correlated quantum system, although details of this control have not been elucidated in many cases. We find that, in the presence of a significant static off-diagonal coupling, quantum coherence can survive much longer than the bath correlation time in a noisy environment. In the presence of time correlated noise (non-Markovian limit), coherence could propagate through the excited bath states, and this plays a nontrivial role in giving rise to a noncanonical temperature dependence of population distribution in an extended conjugated polymer-like system. The quantum coherence through the excited bath states vanishes in the high temperature limit, giving rise to the equilibrium Boltzmann distribution. Second, we discuss a role of quantum coherence in exciton localization that bears resemblance to Anderson localization. Calculations have been carried out not only with a chain of conjugated polymer but also with dimer and trimer subunits of the Fenna−Matthews−Olson (FMO) complex. We derive an analytical expression of the relation between steady state coherence and excitionic population distribution. We analytically showed that steady state coherence in equilibrium bath states is governed by interchromophoric coupling (J) whereas coherence in excited bath states is dictated by fluctuation strength (V d ) for the spatially correlated bath model. For the spatially uncorrelated bath model, we observe that at the low temperature limit coherence in the excited bath states dominates over coherence in equilibrium bath states and vice versa. In the study of the localization problem, we analytically show that, in the limit of a negligibly small fluctuation rate (b d ), the diffusion coefficient is exactly proportional to the fluctuation rate, leading to complete breakdown of the Haken−Strobl−Silbey Markovian prediction.

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Delocalization and Quantum Entanglement in Physical Systems

Cited by 7 publications

References 39 publications

Excitation Energy Transfer Efficiency in Fluctuating Environments: Role of Quantum Coherence in the Presence of Memory Effects

Excitation Energy Transfer Efficiency in Fluctuating Environments: Role of Quantum Coherence in the Presence of Memory Effects

Importance of Intermonomer Couplings of the FMO Complex in Coherently Initiated Dynamics

Quantum Coherence and Its Signatures in Extended Quantum Systems

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