Tensor Network Path Integral Study of Dynamics in B850 LH2 Ring with Atomistically Derived Vibrations

In this mini review, we focus on recent advances in the atomistic modeling of biological light-harvesting (LH) complexes. Because of their size and sophisticated electronic structures, multiscale methods are required to investigate the dynamical and spectroscopic properties of such complexes. The excitation energies, in this context also known as site energies, excitonic couplings, and spectral densities are key quantities which usually need to be extracted to be able to determine the exciton dynamics and spectroscopic properties. The recently developed multiscale approach based on the numerically efficient density functional tight-binding framework followed by excited state calculations has been shown to be superior to the scheme based on pure classical molecular dynamics simulations. The enhanced approach, which improves the description of the internal vibrational dynamics of the pigment molecules, yields spectral densities in good agreement with the experimental counterparts for various bacterial and plant LH systems. Here, we provide a brief overview of those results and described the theoretical foundation of the multiscale protocol.

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“… 2011 ; Mühlbacher and Kleinekathöfer 2012 ; Jansen 2021 ; Varvelo et al. 2021 ; Kundu and Makri 2022 ; Bose and Walters 2022 ).…”

Section: Discussionunclassified

Recent progress in atomistic modeling of light-harvesting complexes: a mini review

Maity

Kleinekathöfer

2022

Photosynth Res

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“…[9][10][11][12] These ideas have also been successfully extended to a multisite framework capable of simulating the quantum dynamics of extended systems coupled with local dissipative media. [13][14][15] Despite the power and novelty of the methods discussed till now, they are unable to provide a clear and unambiguous insight into the mechanism of the transport. Consider an extended system with a non-trivial topology allowing for long-ranged couplings between sites, and assume we are interested in the transport of an exciton.…”

Section: Introductionmentioning

confidence: 99%

Impact of solvent on state-to-state population transport in multistate systems using coherences

Bose¹,

Walters²

2023

Preprint

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We present an approach of analyzing the transport of a quantum particle in a non-trivially connected extended system interacting with a dissipative medium. There are broadly two different aspects of the problem that affect the route taken by the transport process. First is obviously the couplings between the various sites, which translates into the intrinsic "strength" of a channel. Apart from the inter-site couplings, the solvents affecting the energies of the sites, and their relative coupling strengths and time-scales form the second factor. This impact of the such dissipative media is significantly more difficult to analyze. The Channel-Dependent Population Transfer (CDPT) method of analyzing the transport allows us to account for both the effects in a rigorous manner. We demonstrate the richness hidden behind the transport even for relatively simple systems -the effect of the local dissipative media is highly non-trivial and can mask the simplicity of the effect of the relative magnitude of the inter-site couplings. This opens up possibilities in terms of detailed study of the impact of factors on the nature of dynamics, especially possibilities of design of novel systems with an eye towards quantum control.

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“…MS-TNPI is able to simulate the dynamics of open, extended quantum systems accounting for non-Markovian memory. This has been used advantageously to simulate the excitonic dynamics in photosynthetic complexes [26].…”

Section: Introductionmentioning

confidence: 99%

Effect of Phonons and Impurities on the Quantum Transport in XXZ Spin-Chains

Bose¹

2022

Preprint

Self Cite

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Numerical and analytic results have been used to characterize quantum transport in spin chains, showing the existence of both ballistic and diffusive motion. Experiments have shown that heat transfer is surprisingly always diffusive. The scattering from phonons and impurities have been postulated to be the two factors critical in causing the diffusive transport. In this work, we evaluate the transport process by incorporating a bath of phonons and impurities in order to understand the role played by each of the factors. While methods like time-dependent density matrix renormalization group (tDMRG) can be used to simulate isolated spin chains, the coupling with phonons make simulations significantly more challenging. The recently developed multisite tensor network path integral (MS-TNPI) method builds a framework for simulating the dynamics in extended open quantum systems by combining ideas from tDMRG and Feynman-Vernon influence functional. This MS-TNPI is used to characterize dynamics in open, extended quantum systems. Simulations are done with the commonly used sub-Ohmic, Ohmic and super-Ohmic spectral densities describing the phononic bath. We show that while the transport in presence of impurities eventually becomes diffusive, the exact details are dependent on the specifics of the interactions and amount of impurities. In contrast, the presence of a bath makes the transport diffusive irrespective of the parameters characterizing the bath.

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Tensor Network Path Integral Study of Dynamics in B850 LH2 Ring with Atomistically Derived Vibrations

Cited by 18 publications

References 56 publications

Recent progress in atomistic modeling of light-harvesting complexes: a mini review

Recent progress in atomistic modeling of light-harvesting complexes: a mini review

Impact of solvent on state-to-state population transport in multistate systems using coherences

Effect of Phonons and Impurities on the Quantum Transport in XXZ Spin-Chains

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