Environmentally improved coherent light harvesting

Stefano Tomasi; Dominic M. Rouse; Erik M. Gauger; Brendon W. Lovett; Ivan Kassal

doi:10.1021/acs.jpclett.1c01303

Environmentally improved coherent light harvesting

Stefano Tomasi
, Dominic M. Rouse
, Erik M. Gauger
, Brendon W. Lovett
, Ivan Kassal

Research output: Contribution to journal › Article › peer-review

Abstract

Coherence-enhanced light harvesting has not been directly observed experimentally, despite theoretical evidence that coherence can significantly enhance light-harvesting performance. The main experimental obstacle has been the difficulty in isolating the effect of coherence in the presence of confounding variables. Recent proposals for externally controlling coherence by manipulating the light’s degree of polarization showed that coherent efficiency enhancements would be possible, but they were restricted to light-harvesting systems weakly coupled to their environment. Here, we show that increases in system–bath coupling strength can amplify coherent efficiency enhancements, rather than suppress them. This result dramatically broadens the range of systems that could be used to conclusively demonstrate coherence-enhanced light harvesting or to engineer coherent effects into artificial light-harvesting devices.

Original language	English
Pages (from-to)	6143-6151
Number of pages	9
Journal	Journal of Physical Chemistry Letters
Volume	12
Early online date	28 Jun 2021
DOIs	https://doi.org/10.1021/acs.jpclett.1c01303
Publication status	Published - 8 Jul 2021

Keywords

Excitons
Polarons
Light
Energy
Quantum mechanics

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Tomasi_2021_JPL_Environmentally-improved_AAM
Copyright © 2021 American Chemical Society. This work has been made available online in accordance with publisher policies or with permission. Permission for further reuse of this content should be sought from the publisher or the rights holder. This is the author created accepted manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at https://doi.org/10.1021/acs.jpclett.1c01303.
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The effects of strong environmental coupling on light-harvesting systems
Rouse, D. M. (Author), Lovett, B. W. (Supervisor) & Gauger, E. M. (Supervisor), 29 Nov 2022
Student thesis: Doctoral Thesis (PhD)

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title = "Environmentally improved coherent light harvesting",

abstract = "Coherence-enhanced light harvesting has not been directly observed experimentally, despite theoretical evidence that coherence can significantly enhance light-harvesting performance. The main experimental obstacle has been the difficulty in isolating the effect of coherence in the presence of confounding variables. Recent proposals for externally controlling coherence by manipulating the light{\textquoteright}s degree of polarization showed that coherent efficiency enhancements would be possible, but they were restricted to light-harvesting systems weakly coupled to their environment. Here, we show that increases in system{\textendash}bath coupling strength can amplify coherent efficiency enhancements, rather than suppress them. This result dramatically broadens the range of systems that could be used to conclusively demonstrate coherence-enhanced light harvesting or to engineer coherent effects into artificial light-harvesting devices.",

keywords = "Excitons, Polarons, Light, Energy, Quantum mechanics",

author = "Stefano Tomasi and Rouse, \{Dominic M.\} and Gauger, \{Erik M.\} and Lovett, \{Brendon W.\} and Ivan Kassal",

note = "Funding: S.T. and I.K. were supported by a Westpac Scholars Trust Research Fellowship, by an Australian Government Research Training Program scholarship, by the University of Sydney Nano Institute Grand Challenge Computational Materials Discovery, and by computational resources from the National Computational Infrastructure and the Sydney Informatics Hub. D.M.R. acknowledges studentship funding from EPSRC Grant EP/L015110/1, and E.M.G. acknowledges EPSRC Grant EP/T007214/1. ",

year = "2021",

month = jul,

day = "8",

doi = "10.1021/acs.jpclett.1c01303",

language = "English",

volume = "12",

pages = "6143--6151",

journal = "Journal of Physical Chemistry Letters",

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publisher = "American Chemical Society (ACS)",

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T1 - Environmentally improved coherent light harvesting

AU - Tomasi, Stefano

AU - Rouse, Dominic M.

AU - Gauger, Erik M.

AU - Lovett, Brendon W.

AU - Kassal, Ivan

N1 - Funding: S.T. and I.K. were supported by a Westpac Scholars Trust Research Fellowship, by an Australian Government Research Training Program scholarship, by the University of Sydney Nano Institute Grand Challenge Computational Materials Discovery, and by computational resources from the National Computational Infrastructure and the Sydney Informatics Hub. D.M.R. acknowledges studentship funding from EPSRC Grant EP/L015110/1, and E.M.G. acknowledges EPSRC Grant EP/T007214/1.

PY - 2021/7/8

Y1 - 2021/7/8

N2 - Coherence-enhanced light harvesting has not been directly observed experimentally, despite theoretical evidence that coherence can significantly enhance light-harvesting performance. The main experimental obstacle has been the difficulty in isolating the effect of coherence in the presence of confounding variables. Recent proposals for externally controlling coherence by manipulating the light’s degree of polarization showed that coherent efficiency enhancements would be possible, but they were restricted to light-harvesting systems weakly coupled to their environment. Here, we show that increases in system–bath coupling strength can amplify coherent efficiency enhancements, rather than suppress them. This result dramatically broadens the range of systems that could be used to conclusively demonstrate coherence-enhanced light harvesting or to engineer coherent effects into artificial light-harvesting devices.

AB - Coherence-enhanced light harvesting has not been directly observed experimentally, despite theoretical evidence that coherence can significantly enhance light-harvesting performance. The main experimental obstacle has been the difficulty in isolating the effect of coherence in the presence of confounding variables. Recent proposals for externally controlling coherence by manipulating the light’s degree of polarization showed that coherent efficiency enhancements would be possible, but they were restricted to light-harvesting systems weakly coupled to their environment. Here, we show that increases in system–bath coupling strength can amplify coherent efficiency enhancements, rather than suppress them. This result dramatically broadens the range of systems that could be used to conclusively demonstrate coherence-enhanced light harvesting or to engineer coherent effects into artificial light-harvesting devices.

KW - Excitons

KW - Polarons

KW - Light

KW - Energy

KW - Quantum mechanics

U2 - 10.1021/acs.jpclett.1c01303

DO - 10.1021/acs.jpclett.1c01303

M3 - Article

SN - 1948-7185

VL - 12

SP - 6143

EP - 6151

JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

ER -

Environmentally improved coherent light harvesting

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Student theses

The effects of strong environmental coupling on light-harvesting systems

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