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How Static Disorder Mimics Decoherence in Anisotropy Pump-Probe Experiments on Purple-Bacteria Light Harvesting Complexes

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How Static Disorder Mimics Decoherence in Anisotropy Pump-Probe Experiments on Purple-Bacteria Light Harvesting Complexes. / Stross, Clem; Van der Kamp, Marc; Oliver, Thomas A A; Harvey, Jeremy; Linden, Noah; Manby, Fred.

In: Journal of Physical Chemistry B, Vol. 120, No. 44, 10.11.2016, p. 11449-11463.

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@article{af3f6c3aa0a44469bb52b85881ab4e27,
title = "How Static Disorder Mimics Decoherence in Anisotropy Pump-Probe Experiments on Purple-Bacteria Light Harvesting Complexes",
abstract = "Anisotropy pump-probe experiments have provided insights into the character of excitons formed in photosynthetic complexes. Rapid decay in the observed anisotropy is cited as evidence of the strength of coupling of the excitonic degrees of freedom to their environment. Here we show that ensemble averaging over realistic model Hamiltonians leads to a rapid decay of anisotropy to a value close to the observed asymptote, and at a rate comparable to observed decay rates, even in the absence of coupling to the environment. While coupling to the environment will clearly play a role in the dynamics of such systems, our calculations suggest that caution is needed in deducing the strength of this coupling from anisotropy experiments. We also set out to clarify the nature quantum states and processes involved in the dynamics of such systems, and the associated terminology.",
author = "Clem Stross and {Van der Kamp}, Marc and Oliver, {Thomas A A} and Jeremy Harvey and Noah Linden and Fred Manby",
year = "2016",
month = "11",
day = "10",
doi = "10.1021/acs.jpcb.6b09916",
language = "English",
volume = "120",
pages = "11449--11463",
journal = "Journal of Physical Chemistry B",
issn = "1520-6106",
publisher = "American Chemical Society",
number = "44",

}

RIS - suitable for import to EndNote

TY - JOUR

T1 - How Static Disorder Mimics Decoherence in Anisotropy Pump-Probe Experiments on Purple-Bacteria Light Harvesting Complexes

AU - Stross, Clem

AU - Van der Kamp, Marc

AU - Oliver, Thomas A A

AU - Harvey, Jeremy

AU - Linden, Noah

AU - Manby, Fred

PY - 2016/11/10

Y1 - 2016/11/10

N2 - Anisotropy pump-probe experiments have provided insights into the character of excitons formed in photosynthetic complexes. Rapid decay in the observed anisotropy is cited as evidence of the strength of coupling of the excitonic degrees of freedom to their environment. Here we show that ensemble averaging over realistic model Hamiltonians leads to a rapid decay of anisotropy to a value close to the observed asymptote, and at a rate comparable to observed decay rates, even in the absence of coupling to the environment. While coupling to the environment will clearly play a role in the dynamics of such systems, our calculations suggest that caution is needed in deducing the strength of this coupling from anisotropy experiments. We also set out to clarify the nature quantum states and processes involved in the dynamics of such systems, and the associated terminology.

AB - Anisotropy pump-probe experiments have provided insights into the character of excitons formed in photosynthetic complexes. Rapid decay in the observed anisotropy is cited as evidence of the strength of coupling of the excitonic degrees of freedom to their environment. Here we show that ensemble averaging over realistic model Hamiltonians leads to a rapid decay of anisotropy to a value close to the observed asymptote, and at a rate comparable to observed decay rates, even in the absence of coupling to the environment. While coupling to the environment will clearly play a role in the dynamics of such systems, our calculations suggest that caution is needed in deducing the strength of this coupling from anisotropy experiments. We also set out to clarify the nature quantum states and processes involved in the dynamics of such systems, and the associated terminology.

UR - http://doi.org/10.5523/bris.1bhb3c1po4yfu1tsjrbez1s3ce

U2 - 10.1021/acs.jpcb.6b09916

DO - 10.1021/acs.jpcb.6b09916

M3 - Article

VL - 120

SP - 11449

EP - 11463

JO - Journal of Physical Chemistry B

T2 - Journal of Physical Chemistry B

JF - Journal of Physical Chemistry B

SN - 1520-6106

IS - 44

ER -