Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Coherent quantum transport in disordered systems: A unified polaron treatment of hopping and band-like transport

Abstract

Quantum transport in disordered systems is studied using a polaron-based master equation. The polaron approach is capable of bridging the results from the coherent band-like transport regime governed by the Redfield equation to incoherent hopping transport in the classical regime. Additionally, a non-monotonic dependence of the diffusion coefficient is observed both as a function of temperature and system-phonon coupling strength. In the band-like transport regime, the diffusion coefficient is shown to be linearly proportional to the system-phonon coupling strength and vanishes at zero coupling due to Anderson localization. In the opposite classical hopping regime, we correctly recover the dynamics described by the Fermi’s Golden Rule and establish that the scaling of the diffusion coefficient depends on the phonon bath relaxation time. In both the hopping and band-like transport regimes, it is demonstrated that at low temperature, the zero-point fluctuations of the bath lead to non-zero transport rates and hence a finite diffusion constant. Lastly, application to rubrene and other organic semiconductor materials shows a good agreement with experimental mobility data.

Authors:
 [1];  [2];  [2]
+ Show Author Affiliations
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); National Univ. of Singapore (Singapore)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Publication Date:
Research Org.:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1546992
Alternate Identifier(s):
OSTI ID: 1228308
Grant/Contract Number:  
SC0001088
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 142; Journal Issue: 16; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Lee, Chee Kong, Moix, Jeremy, and Cao, Jianshu. Coherent quantum transport in disordered systems: A unified polaron treatment of hopping and band-like transport. United States: N. p., 2015. Web. doi:10.1063/1.4918736.
Copy to clipboard
Lee, Chee Kong, Moix, Jeremy, & Cao, Jianshu. Coherent quantum transport in disordered systems: A unified polaron treatment of hopping and band-like transport. United States. https://doi.org/10.1063/1.4918736
Copy to clipboard
Lee, Chee Kong, Moix, Jeremy, and Cao, Jianshu. Fri . "Coherent quantum transport in disordered systems: A unified polaron treatment of hopping and band-like transport". United States. https://doi.org/10.1063/1.4918736. https://www.osti.gov/servlets/purl/1546992.
Copy to clipboard
@article{osti_1546992,
title = {Coherent quantum transport in disordered systems: A unified polaron treatment of hopping and band-like transport},
author = {Lee, Chee Kong and Moix, Jeremy and Cao, Jianshu},
abstractNote = {Quantum transport in disordered systems is studied using a polaron-based master equation. The polaron approach is capable of bridging the results from the coherent band-like transport regime governed by the Redfield equation to incoherent hopping transport in the classical regime. Additionally, a non-monotonic dependence of the diffusion coefficient is observed both as a function of temperature and system-phonon coupling strength. In the band-like transport regime, the diffusion coefficient is shown to be linearly proportional to the system-phonon coupling strength and vanishes at zero coupling due to Anderson localization. In the opposite classical hopping regime, we correctly recover the dynamics described by the Fermi’s Golden Rule and establish that the scaling of the diffusion coefficient depends on the phonon bath relaxation time. In both the hopping and band-like transport regimes, it is demonstrated that at low temperature, the zero-point fluctuations of the bath lead to non-zero transport rates and hence a finite diffusion constant. Lastly, application to rubrene and other organic semiconductor materials shows a good agreement with experimental mobility data.},
doi = {10.1063/1.4918736},
journal = {Journal of Chemical Physics},
number = 16,
volume = 142,
place = {United States},
year = {Fri Apr 24 00:00:00 EDT 2015},
month = {Fri Apr 24 00:00:00 EDT 2015}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1063/1.4918736
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 48 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Theoretical description of quantum effects in multi-chromophoric aggregates
journal, August 2012

  • Zimanyi, Eric N.; Silbey, Robert J.
  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 370, Issue 1972
  • DOI: 10.1098/rsta.2011.0204

A unified theory for charge-carrier transport in organic crystals
journal, March 2008

  • Cheng, Yuan-Chung; Silbey, Robert J.
  • The Journal of Chemical Physics, Vol. 128, Issue 11
  • DOI: 10.1063/1.2894840

Optimization of Exciton Trapping in Energy Transfer Processes
journal, December 2009

  • Cao, Jianshu; Silbey, Robert J.
  • The Journal of Physical Chemistry A, Vol. 113, Issue 50
  • DOI: 10.1021/jp9032589

Conformational Disorder and Ultrafast Exciton Relaxation in PPV-family Conjugated Polymers
journal, January 2009

  • Dykstra, Tieneke E.; Hennebicq, Emmanuelle; Beljonne, David
  • The Journal of Physical Chemistry B, Vol. 113, Issue 3
  • DOI: 10.1021/jp807249b

Charge Transport in Organic Semiconductors
journal, April 2007

  • Coropceanu, Veaceslav; Cornil, Jérôme; da Silva Filho, Demetrio A.
  • Chemical Reviews, Vol. 107, Issue 4
  • DOI: 10.1021/cr050140x

Band-like temperature dependence of mobility in a solution-processed organic semiconductor
journal, August 2010

  • Sakanoue, Tomo; Sirringhaus, Henning
  • Nature Materials, Vol. 9, Issue 9
  • DOI: 10.1038/nmat2825

Low-temperature dynamics of weakly localized Frenkel excitons in disordered linear chains
journal, February 2004

  • Bednarz, M.; Malyshev, V. A.; Knoester, J.
  • The Journal of Chemical Physics, Vol. 120, Issue 8
  • DOI: 10.1063/1.1643720

Electronic excitation dynamics in multichromophoric systems described via a polaron-representation master equation
journal, October 2011

  • Kolli, Avinash; Nazir, Ahsan; Olaya-Castro, Alexandra
  • The Journal of Chemical Physics, Vol. 135, Issue 15
  • DOI: 10.1063/1.3652227

Transient localization in crystalline organic semiconductors
journal, February 2011

Exciton Migration in Molecular Crystals
journal, June 1971

  • Grover, M.; Silbey, R.
  • The Journal of Chemical Physics, Vol. 54, Issue 11
  • DOI: 10.1063/1.1674761

Anisotropic field effect mobility in single crystal pentacene
journal, June 2006

  • Lee, J. Y.; Roth, S.; Park, Y. W.
  • Applied Physics Letters, Vol. 88, Issue 25
  • DOI: 10.1063/1.2216400

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

  • Ishizaki, Akihito; Fleming, Graham R.
  • The Journal of Chemical Physics, Vol. 130, Issue 23
  • DOI: 10.1063/1.3155214

Fluorescence depolarization in poly[2-methoxy-5-((2-ethylhexyl)oxy)-1,4-phenylenevinylene]: Sites versus eigenstates hopping
journal, January 2009

  • Singh, Jaykrishna; Bittner, Eric R.; Beljonne, David
  • The Journal of Chemical Physics, Vol. 131, Issue 19
  • DOI: 10.1063/1.3259549

Theory of multichromophoric coherent resonance energy transfer: A polaronic quantum master equation approach
journal, July 2011

  • Jang, Seogjoo
  • The Journal of Chemical Physics, Vol. 135, Issue 3
  • DOI: 10.1063/1.3608914

Criteria for the accuracy of small polaron quantum master equation in simulating excitation energy transfer dynamics
journal, December 2013

  • Chang, Hung-Tzu; Zhang, Pan-Pan; Cheng, Yuan-Chung
  • The Journal of Chemical Physics, Vol. 139, Issue 22
  • DOI: 10.1063/1.4840795

A Structure-Based Model of Energy Transfer Reveals the Principles of Light Harvesting in Photosystem II Supercomplexes
journal, June 2013

  • Bennett, Doran I. G.; Amarnath, Kapil; Fleming, Graham R.
  • Journal of the American Chemical Society, Vol. 135, Issue 24
  • DOI: 10.1021/ja403685a

First-principles calculations of anisotropic charge-carrier mobilities in organic semiconductor crystals
journal, April 2011

Efficient Energy Transfer in Light-Harvesting Systems, III: The Influence of the Eighth Bacteriochlorophyll on the Dynamics and Efficiency in FMO
journal, November 2011

  • Moix, Jeremy; Wu, Jianlan; Huo, Pengfei
  • The Journal of Physical Chemistry Letters, Vol. 2, Issue 24
  • DOI: 10.1021/jz201259v

Temperature Dependent Fluorescence in Disordered Frenkel Chains: Interplay of Equilibration and Local Band-Edge Level Structure
journal, November 2003

Damping of Exciton Rabi Rotations by Acoustic Phonons in Optically Excited InGaAs / GaAs Quantum Dots
journal, January 2010

Variational calculation of the dynamics of a two level system interacting with a bath
journal, March 1984

  • Silbey, Robert; Harris, Robert A.
  • The Journal of Chemical Physics, Vol. 80, Issue 6
  • DOI: 10.1063/1.447055

Coherence Dynamics in Photosynthesis: Protein Protection of Excitonic Coherence
journal, June 2007

Theory of charge transport in organic crystals: Beyond Holstein’s small-polaron model
journal, June 2009

Intrinsic Charge Transport on the Surface of Organic Semiconductors
journal, August 2004

Quantum Transport of Slow Charge Carriers in Quasicrystals and Correlated Systems
journal, July 2006

A multi-site variational master equation approach to dissipative energy transfer
journal, July 2013

Relaxation Dynamics of Photoexcited Excitons in Rubrene Single Crystals Using Femtosecond Absorption Spectroscopy
journal, August 2012

Multi-quanta energy relaxation in a nonlinear quantum dimer coupled to a phonon bath
journal, September 2006

Charge-Transport Regime of Crystalline Organic Semiconductors: Diffusion Limited by Thermal Off-Diagonal Electronic Disorder
journal, March 2006

Accuracy of second order perturbation theory in the polaron and variational polaron frames
journal, May 2012

  • Lee, Chee Kong; Moix, Jeremy; Cao, Jianshu
  • The Journal of Chemical Physics, Vol. 136, Issue 20
  • DOI: 10.1063/1.4722336

Coherent and incoherent dynamics in excitonic energy transfer: Correlated fluctuations and off-resonance effects
journal, April 2011

Elastomeric Transistor Stamps: Reversible Probing of Charge Transport in Organic Crystals
journal, March 2004

  • Sundar, Vikram C.; Zaumseil, Jana; Podzorov, Vitaly
  • Science, Vol. 303, Issue 5664, p. 1644-1646
  • DOI: 10.1126/science.1094196

Theory of coherent resonance energy transfer
journal, September 2008

  • Jang, Seogjoo; Cheng, Yuan-Chung; Reichman, David R.
  • The Journal of Chemical Physics, Vol. 129, Issue 10
  • DOI: 10.1063/1.2977974

Nonequilibrium Energy Transfer at Nanoscale: A Unified Theory from Weak to Strong Coupling
journal, July 2015

  • Wang, Chen; Ren, Jie; Cao, Jianshu
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep11787

Charge Transport in Organic Semiconductors
journal, July 2007

  • Coropceanu, Veaceslav; Cornil, Jerome; da Silva Filho, Demetrio A.
  • ChemInform, Vol. 38, Issue 29
  • DOI: 10.1002/chin.200729266

A multi-site variational master equation approach to dissipative energy transfer
text, January 2012

Intrinsic charge transport on the surface of organic semiconductors
text, January 2004

Quantum transport of slow charge carriers in quasicrystals and correlated systems
text, January 2006

    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Nonequilibrium Energy Transfer at Nanoscale: A Unified Theory from Weak to Strong Coupling
    journal, July 2015

    • Wang, Chen; Ren, Jie; Cao, Jianshu
    • Scientific Reports, Vol. 5, Issue 1
    • DOI: 10.1038/srep11787

    Simulations of infrared and Raman spectra in solution using the fragment molecular orbital method
    journal, January 2019

    • Nakata, Hiroya; Fedorov, Dmitri G.
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 25
    • DOI: 10.1039/c9cp00940j

    Brownian ratchets: How stronger thermal noise can reduce diffusion
    journal, February 2017

    • Spiechowicz, Jakub; Kostur, Marcin; Łuczka, Jerzy
    • Chaos: An Interdisciplinary Journal of Nonlinear Science, Vol. 27, Issue 2
    • DOI: 10.1063/1.4976586

    Modeling the effects of molecular disorder on the properties of Frenkel excitons in organic molecular semiconductors
    journal, September 2018

    • Shi, Liang; Willard, Adam P.
    • The Journal of Chemical Physics, Vol. 149, Issue 9
    • DOI: 10.1063/1.5044553

    Polaron effects on the performance of light-harvesting systems: a quantum heat engine perspective
    journal, January 2016

    Describing many-body localized systems in thermal environments
    journal, June 2019

    • Wu, Ling-Na; Schnell, Alexander; Tomasi, Giuseppe De
    • New Journal of Physics, Vol. 21, Issue 6
    • DOI: 10.1088/1367-2630/ab25a4

    Unifying quantum heat transfer in a nonequilibrium spin-boson model with full counting statistics
    journal, February 2017

    Steady-state entanglement and coherence of two coupled qubits in equilibrium and nonequilibrium environments
    journal, April 2019

    Polaron relaxation and charge dynamics near the mobility edge of a possible Wigner lattice of polarons
    journal, July 2018

    • Hettiarachchi, Gayan Prasad; Nishida, Yoshifumi; Masaki, Yusuke
    • Physical Review B, Vol. 98, Issue 3
    • DOI: 10.1103/physrevb.98.035125

    Quantum Diffusion on Molecular Tubes: Universal Scaling of the 1D to 2D Transition
    journal, May 2016

    Brownian ratchets: How stronger thermal noise can reduce diffusion
    text, January 2017

    Nonequilibrium Energy Transfer at Nanoscale: A Unified Theory from Weak to Strong Coupling
    journal, July 2015

    • Wang, Chen; Ren, Jie; Cao, Jianshu
    • Scientific Reports, Vol. 5, Issue 1
    • DOI: 10.1038/srep11787

    Molecular dynamics and charge transport in organic semiconductors: a classical approach to modeling electron transfer
    journal, January 2017

    • Pelzer, Kenley M.; Vázquez-Mayagoitia, Álvaro; Ratcliff, Laura E.
    • Chemical Science, Vol. 8, Issue 4
    • DOI: 10.1039/c6sc04547b
      Sort by:
      [ × clear filter / sort ]

      Similar Records in DOE PAGES and OSTI.GOV collections: