Disorder-Induced Quantum Beats in Two-Dimensional Spectra of Excitonically Coupled Molecules

Butkus, Vytautas; Dong, Hui; Fleming, Graham R.; Abramavicius, Darius; Valkunas, Leonas

doi:10.1021/acs.jpclett.5b02642

Title: Disorder-Induced Quantum Beats in Two-Dimensional Spectra of Excitonically Coupled Molecules

Abstract

Here, a study is presented showing the conditions when long-lived electronic quantum coherences originating from recently proposed inhomogeneous broadening mechanism are enhanced and reflected in the two-dimensional electronic spectra of the excitonically coupled molecular dimer. We show that depending on the amount of inhomogeneous broadening, the excitonically coupled molecular system can establish long-lived electronic coherences, caused by a disordered subensemble, for which the dephasing due to static energy disorder becomes significantly reduced. On the basis of these considerations, we present explanations for why the electronic or vibrational coherences were or were not observed in a range of recent experiments.

Authors:: Butkus, Vytautas; Dong, Hui; Fleming, Graham R.; Abramavicius, Darius; Valkunas, Leonas

Publication Date:: Thu Jan 21 00:00:00 EST 2016

Research Org.:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1379226

Grant/Contract Number:: AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry Letters

Additional Journal Information:: Journal Volume: 7; Journal Issue: 2; Journal ID: ISSN 1948-7185

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Butkus, Vytautas, Dong, Hui, Fleming, Graham R., Abramavicius, Darius, and Valkunas, Leonas. Disorder-Induced Quantum Beats in Two-Dimensional Spectra of Excitonically Coupled Molecules.  United States: N. p., 2016. 
Web.  doi:10.1021/acs.jpclett.5b02642.

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                    Butkus, Vytautas, Dong, Hui, Fleming, Graham R., Abramavicius, Darius, & Valkunas, Leonas. Disorder-Induced Quantum Beats in Two-Dimensional Spectra of Excitonically Coupled Molecules.  United States.  https://doi.org/10.1021/acs.jpclett.5b02642

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                    Butkus, Vytautas, Dong, Hui, Fleming, Graham R., Abramavicius, Darius, and Valkunas, Leonas. Thu .  
"Disorder-Induced Quantum Beats in Two-Dimensional Spectra of Excitonically Coupled Molecules".  United States.  https://doi.org/10.1021/acs.jpclett.5b02642.  https://www.osti.gov/servlets/purl/1379226.

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@article{osti_1379226,

  title        = {Disorder-Induced Quantum Beats in Two-Dimensional Spectra of Excitonically Coupled Molecules},

  author       = {Butkus, Vytautas and Dong, Hui and Fleming, Graham R. and Abramavicius, Darius and Valkunas, Leonas},

  abstractNote = {Here, a study is presented showing the conditions when long-lived electronic quantum coherences originating from recently proposed inhomogeneous broadening mechanism are enhanced and reflected in the two-dimensional electronic spectra of the excitonically coupled molecular dimer. We show that depending on the amount of inhomogeneous broadening, the excitonically coupled molecular system can establish long-lived electronic coherences, caused by a disordered subensemble, for which the dephasing due to static energy disorder becomes significantly reduced. On the basis of these considerations, we present explanations for why the electronic or vibrational coherences were or were not observed in a range of recent experiments.},

  doi          = {10.1021/acs.jpclett.5b02642},

  journal      = {Journal of Physical Chemistry Letters},

  number       = 2,

  volume       = 7,

  place        = {United States},

  year         = {Thu Jan 21 00:00:00 EST 2016},

  month        = {Thu Jan 21 00:00:00 EST 2016}

}

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Title: Disorder-Induced Quantum Beats in Two-Dimensional Spectra of Excitonically Coupled Molecules

Abstract

Citation Formats

Theory of Molecular Excitons book, January 1971

Exciton localization in polymers with static disorder journal, October 2009

Photosynthetic Excitons book, January 2000

Theoretical examination of quantum coherence in a photosynthetic system at physiological temperature journal, October 2009

Environment-assisted quantum transport journal, March 2009

M ULTIDIMENSIONAL F EMTOSECOND C ORRELATION S PECTROSCOPIES OF E LECTRONIC AND V IBRATIONAL E XCITATIONS journal, October 2000

Phase-stabilized two-dimensional electronic spectroscopy journal, September 2004

Quantum effects in biology journal, January 2011

Experimental Implementations of Two-Dimensional Fourier Transform Electronic Spectroscopy journal, April 2015

Vibronic phenomena and exciton–vibrational interference in two-dimensional spectra of molecular aggregates journal, January 2014

Coherent Intrachain Energy Migration in a Conjugated Polymer at Room Temperature journal, January 2009

Vibronic coherence in oxygenic photosynthesis journal, July 2014

Quantum coherence in photosynthesis for efficient solar-energy conversion journal, July 2014

Role of coherent vibrations in energy transfer and conversion in photosynthetic pigment–protein complexes journal, January 2015

Coherent Exciton Dynamics in the Presence of Underdamped Vibrations journal, February 2015

Exciton dynamics in chromophore aggregates with correlated environment fluctuations journal, May 2011

Direct evidence of quantum transport in photosynthetic light-harvesting complexes journal, December 2011

Origin of Long-Lived Coherences in Light-Harvesting Complexes journal, June 2012

Distinctive character of electronic and vibrational coherences in disordered molecular aggregates journal, November 2013

Inhomogeneous Broadening Induced Long-Lived Integrated Two-Color Coherence Photon Echo Signal journal, July 2014

T WO -D IMENSIONAL F EMTOSECOND S PECTROSCOPY journal, October 2003

The role of non-equilibrium vibrational structures in electronic coherence and recoherence in pigment–protein complexes journal, January 2013

Coherent Multidimensional Optical Spectroscopy of Excitons in Molecular Aggregates; Quasiparticle versus Supermolecule Perspectives journal, June 2009

On the adequacy of the Redfield equation and related approaches to the study of quantum dynamics in electronic energy transfer journal, June 2009

Combined treatment of relaxation and fluctuation dynamics in the calculation of two-dimensional electronic spectra journal, September 2014

Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems journal, April 2007

Coherent Picosecond Exciton Dynamics in a Photosynthetic Reaction Center journal, October 2012

Role of Electronic-Vibrational Mixing in Enhancing Vibrational Coherences in the Ground Electronic States of Photosynthetic Bacterial Reaction Center journal, January 2014

Two-dimensional spectroscopy of a molecular dimer unveils the effects of vibronic coupling on exciton coherences journal, January 2014

2D Spectroscopy Study of Water-Soluble Chlorophyll-Binding Protein from Lepidium virginicum journal, March 2014

Electronic Couplings and Energy Transfer Dynamics in the Oxidized Primary Electron Donor of the Bacterial Reaction Center journal, February 2004

The Mechanism of Energy Transfer in the Bacterial Photosynthetic Reaction Center journal, March 2001

Electron−Vibrational Coupling in the Fenna−Matthews−Olson Complex of Prosthecochloris aestuarii Determined by Temperature-Dependent Absorption and Fluorescence Line-Narrowing Measurements May 2000

Theory of Molecular Excitons
book, January 1971

Exciton localization in polymers with static disorder
journal, October 2009

Photosynthetic Excitons
book, January 2000

Theoretical examination of quantum coherence in a photosynthetic system at physiological temperature
journal, October 2009

Environment-assisted quantum transport
journal, March 2009

M ULTIDIMENSIONAL F EMTOSECOND C ORRELATION S PECTROSCOPIES OF E LECTRONIC AND V IBRATIONAL E XCITATIONS
journal, October 2000

Phase-stabilized two-dimensional electronic spectroscopy
journal, September 2004

Quantum effects in biology
journal, January 2011

Experimental Implementations of Two-Dimensional Fourier Transform Electronic Spectroscopy
journal, April 2015

Vibronic phenomena and exciton–vibrational interference in two-dimensional spectra of molecular aggregates
journal, January 2014

Coherent Intrachain Energy Migration in a Conjugated Polymer at Room Temperature
journal, January 2009

Vibronic coherence in oxygenic photosynthesis
journal, July 2014

Quantum coherence in photosynthesis for efficient solar-energy conversion
journal, July 2014

Role of coherent vibrations in energy transfer and conversion in photosynthetic pigment–protein complexes
journal, January 2015

Coherent Exciton Dynamics in the Presence of Underdamped Vibrations
journal, February 2015

Exciton dynamics in chromophore aggregates with correlated environment fluctuations
journal, May 2011

Direct evidence of quantum transport in photosynthetic light-harvesting complexes
journal, December 2011

Origin of Long-Lived Coherences in Light-Harvesting Complexes
journal, June 2012

Distinctive character of electronic and vibrational coherences in disordered molecular aggregates
journal, November 2013

Inhomogeneous Broadening Induced Long-Lived Integrated Two-Color Coherence Photon Echo Signal
journal, July 2014

T WO -D IMENSIONAL F EMTOSECOND S PECTROSCOPY
journal, October 2003

The role of non-equilibrium vibrational structures in electronic coherence and recoherence in pigment–protein complexes
journal, January 2013

Coherent Multidimensional Optical Spectroscopy of Excitons in Molecular Aggregates; Quasiparticle versus Supermolecule Perspectives
journal, June 2009

On the adequacy of the Redfield equation and related approaches to the study of quantum dynamics in electronic energy transfer
journal, June 2009

Combined treatment of relaxation and fluctuation dynamics in the calculation of two-dimensional electronic spectra
journal, September 2014

Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems
journal, April 2007

Coherent Picosecond Exciton Dynamics in a Photosynthetic Reaction Center
journal, October 2012

Role of Electronic-Vibrational Mixing in Enhancing Vibrational Coherences in the Ground Electronic States of Photosynthetic Bacterial Reaction Center
journal, January 2014

Two-dimensional spectroscopy of a molecular dimer unveils the effects of vibronic coupling on exciton coherences
journal, January 2014

2D Spectroscopy Study of Water-Soluble Chlorophyll-Binding Protein from Lepidium virginicum
journal, March 2014

Electronic Couplings and Energy Transfer Dynamics in the Oxidized Primary Electron Donor of the Bacterial Reaction Center
journal, February 2004

The Mechanism of Energy Transfer in the Bacterial Photosynthetic Reaction Center
journal, March 2001

Electron−Vibrational Coupling in the Fenna−Matthews−Olson Complex of Prosthecochloris aestuarii Determined by Temperature-Dependent Absorption and Fluorescence Line-Narrowing Measurements
May 2000