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Bulletin of the American Physical Society

Control of Quantum Energy Transport by Environmental Engineering

Chikako Uchiyama

Published Mar 5, 2020• 0 citations
OpenAlex

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Environmental engineering for quantum energy transport

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Transport phenomena are ubiquitous throughout the science, engineering and technology disciplines as it concerns energy, mass, charge and information exchange between systems.In particular, energy transport in the nanoscale regime has attracted significant attention within the physical science community due to its potential to explain complex phenomena like the electronic energy transfer in molecular crystals or the Fenna-Matthews-Olson (FMO) / light harvesting complexes in photosynthetic bacteria with long time coherences.Energy transport in these systems is highly affected by environmental noise but surprisingly not always in a detrimental way.It was recently found that situations exist where noise actually enhances the transport phenomena.Such noise can take many forms, but can be characterised in three basic behaviours: quantum, correlation in time, or space.All have been shown potential to offer an energy transport enhancement.The focus of this work is on quantum transport caused by stochastic environment with spatio-temporal correlation.We consider a multi-site nearest neighbour interaction model with pure dephasing environmental noise with spatio-temporal correlation and show how an accelerated rate for the energy transfer results especially under negative spatial correlation (anti-correlation).Spatial anti-correlation provides another control parameter to help one establish the most efficient transfer of energy and may provide new insights into the working of exciton transport in photosynthetic complexes.Further the usage of spatio-temporal correlated noise may be a beneficial resource for efficient transport in large scale quantum networks.

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Excitation-energy transfer underpins the conversion of light into usable energy in photosynthetic organisms and serves as a paradigm for evolutionary optimized transport in open quantum systems. Although this process is often described as incoherent thermally assisted hopping, such descriptions become inadequate when electronic coupling, vibronic interactions and environmental fluctuations occur on comparable energy scales. Determining how the environment controls transport therefore remains a fundamental challenge. Here, we use temperature-dependent 2DES to investigate energy transfer in the photosynthetic antenna protein allophycocyanin over the range 10 - 296 K. The dominant $β\rightarrow α$ transfer step exhibits a pronounced non-monotonic temperature dependence: the transfer time decreases from 400 fs at 10 K to 200 fs near 30- 40 K before increasing again to 400 fs at 296 K. In contrast, the homogeneous optical dephasing time decreases monotonically across the same temperature range. To interpret these observations, we model APC as a vibronically coupled excitonic dimer interacting with a structured environment and solve the dynamics using hierarchical equations of motion. Conventional fixed-bath models, including Drude-Lorentz and explicit intermolecular-mode spectral densities, fail to reproduce the observed turnover. Quantitative agreement is obtained only when the low-frequency sector of the environmental spectral density is allowed to anharmonically evolve strongly with temperature, while the high-frequency bath remains essentially unchanged. More broadly, these findings demonstrate that transport efficiency is controlled not simply by the magnitude of environmental fluctuations, but by the distribution of environmental spectral weight across frequency space, providing new experimental constraints on theories of molecular transport in complex quantum environments.

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Environmental engineering for quantum energy transport

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Abstract Transport phenomena are ubiquitous throughout the science, engineering, and technology disciplines as it concerns energy, mass, charge, and information exchange between systems. In particular, energy transport in the nanoscale regime has attracted significant attention within the physical science community due to its potential to explain complex phenomena like the electronic energy transfer in molecular crystals or the Fenna-Matthews-Olson (FMO)/light harvesting complexes in photosynthetic bacteria with long time coherences. Energy transport in these systems is highly affected by environmental noise but surprisingly not always in a detrimental way. It was recently found that situations exist where noise actually enhances the transport phenomena. Such noise can take many forms, but can be characterised in three basic behaviors: quantum, correlation in time, or space. All have been shown potential to offer an energy transport enhancement. The focus of this work is on quantum transport caused by stochastic environment with spatio-temporal correlation. We consider a multi-site nearest neighbor interaction model with pure dephasing environmental noise with spatio-temporal correlation and show how an accelerated rate for the energy transfer results especially under negative spatial correlation (anti-correlation). Spatial anti-correlation provides another control parameter to help one establish the most efficient transfer of energy and may provide new insights into the working of exciton transport in photosynthetic complexes. Further the usage of spatio-temporal correlated noise may be a beneficial resource for efficient transport in large scale quantum networks.

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Transport phenomena are ubiquitous throughout the science, engineering and technology disciplines as it concerns energy, mass, charge and information exchange between systems.In particular, energy transport in the nanoscale regime has attracted significant attention within the physical science community due to its potential to explain complex phenomena like the electronic energy transfer in molecular crystals or the Fenna-Matthews-Olson (FMO) / light harvesting complexes in photosynthetic bacteria with long time coherences.Energy transport in these systems is highly affected by environmental noise but surprisingly not always in a detrimental way.It was recently found that situations exist where noise actually enhances the transport phenomena.Such noise can take many forms, but can be characterised in three basic behaviours: quantum, correlation in time, or space.All have been shown potential to offer an energy transport enhancement.The focus of this work is on quantum transport caused by stochastic environment with spatio-temporal correlation.We consider a multi-site nearest neighbour interaction model with pure dephasing environmental noise with spatio-temporal correlation and show how an accelerated rate for the energy transfer results especially under negative spatial correlation (anti-correlation).Spatial anti-correlation provides another control parameter to help one establish the most efficient transfer of energy and may provide new insights into the working of exciton transport in photosynthetic complexes.Further the usage of spatio-temporal correlated noise may be a beneficial resource for efficient transport in large scale quantum networks.
Excitation-energy transfer underpins the conversion of light into usable energy in photosynthetic organisms and serves as a paradigm for evolutionary optimized transport in open quantum systems. Although this process is often described as incoherent thermally assisted hopping, such descriptions become inadequate when electronic coupling, vibronic interactions and environmental fluctuations occur on comparable energy scales. Determining how the environment controls transport therefore remains a fundamental challenge. Here, we use temperature-dependent 2DES to investigate energy transfer in the photosynthetic antenna protein allophycocyanin over the range 10 - 296 K. The dominant β→αβ\rightarrow αβ→α transfer step exhibits a pronounced non-monotonic temperature dependence: the transfer time decreases from 400 fs at 10 K to 200 fs near 30- 40 K before increasing again to 400 fs at 296 K. In contrast, the homogeneous optical dephasing time decreases monotonically across the same temperature range. To interpret these observations, we model APC as a vibronically coupled excitonic dimer interacting with a structured environment and solve the dynamics using hierarchical equations of motion. Conventional fixed-bath models, including Drude-Lorentz and explicit intermolecular-mode spectral densities, fail to reproduce the observed turnover. Quantitative agreement is obtained only when the low-frequency sector of the environmental spectral density is allowed to anharmonically evolve strongly with temperature, while the high-frequency bath remains essentially unchanged. More broadly, these findings demonstrate that transport efficiency is controlled not simply by the magnitude of environmental fluctuations, but by the distribution of environmental spectral weight across frequency space, providing new experimental constraints on theories of molecular transport in complex quantum environments.
Abstract Transport phenomena are ubiquitous throughout the science, engineering, and technology disciplines as it concerns energy, mass, charge, and information exchange between systems. In particular, energy transport in the nanoscale regime has attracted significant attention within the physical science community due to its potential to explain complex phenomena like the electronic energy transfer in molecular crystals or the Fenna-Matthews-Olson (FMO)/light harvesting complexes in photosynthetic bacteria with long time coherences. Energy transport in these systems is highly affected by environmental noise but surprisingly not always in a detrimental way. It was recently found that situations exist where noise actually enhances the transport phenomena. Such noise can take many forms, but can be characterised in three basic behaviors: quantum, correlation in time, or space. All have been shown potential to offer an energy transport enhancement. The focus of this work is on quantum transport caused by stochastic environment with spatio-temporal correlation. We consider a multi-site nearest neighbor interaction model with pure dephasing environmental noise with spatio-temporal correlation and show how an accelerated rate for the energy transfer results especially under negative spatial correlation (anti-correlation). Spatial anti-correlation provides another control parameter to help one establish the most efficient transfer of energy and may provide new insights into the working of exciton transport in photosynthetic complexes. Further the usage of spatio-temporal correlated noise may be a beneficial resource for efficient transport in large scale quantum networks.