skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Charge transport network dynamics in molecular aggregates

Abstract

Due to the nonperiodic nature of charge transport in disordered systems, generating insight into static charge transport networks, as well as analyzing the network dynamics, can be challenging. Here, we apply time-dependent network analysis to scrutinize the charge transport networks of two representative molecular semiconductors: a rigid n-type molecule, perylenediimide, and a flexible p-type molecule, b B D T ( T D P P ) 2 . Simulations reveal the relevant timescale for local transfer integral decorrelation to be 100 fs, which is shown to be faster than that of a crystalline morphology of the same molecule. Using a simple graph metric, global network changes are observed over timescales competitive with charge carrier lifetimes. These insights demonstrate that static charge transport networks are qualitatively inadequate, whereas average networks often overestimate network connectivity. Finally, a simple methodology for tracking dynamic charge transport properties is proposed.

Authors:
; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1267525
Alternate Identifier(s):
OSTI ID: 1388188
Grant/Contract Number:  
DC-SC0001059; SC0001059
Resource Type:
Journal Article: Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 113 Journal Issue: 31; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; catalysis (homogeneous); catalysis (heterogeneous); solar (photovoltaic); solar (fuels); photosynthesis (natural and artificial); bio-inspired; hydrogen and fuel cells; electrodes - solar; defects; charge transport; spin dynamics; membrane; materials and chemistry by design; optics; synthesis (novel materials); synthesis (self-assembly)

Citation Formats

Jackson, Nicholas E., Chen, Lin X., and Ratner, Mark A. Charge transport network dynamics in molecular aggregates. United States: N. p., 2016. Web. doi:10.1073/pnas.1601915113.
Jackson, Nicholas E., Chen, Lin X., & Ratner, Mark A. Charge transport network dynamics in molecular aggregates. United States. https://doi.org/10.1073/pnas.1601915113
Jackson, Nicholas E., Chen, Lin X., and Ratner, Mark A. Wed . "Charge transport network dynamics in molecular aggregates". United States. https://doi.org/10.1073/pnas.1601915113.
@article{osti_1267525,
title = {Charge transport network dynamics in molecular aggregates},
author = {Jackson, Nicholas E. and Chen, Lin X. and Ratner, Mark A.},
abstractNote = {Due to the nonperiodic nature of charge transport in disordered systems, generating insight into static charge transport networks, as well as analyzing the network dynamics, can be challenging. Here, we apply time-dependent network analysis to scrutinize the charge transport networks of two representative molecular semiconductors: a rigid n-type molecule, perylenediimide, and a flexible p-type molecule, b B D T ( T D P P ) 2 . Simulations reveal the relevant timescale for local transfer integral decorrelation to be ∼ 100 fs, which is shown to be faster than that of a crystalline morphology of the same molecule. Using a simple graph metric, global network changes are observed over timescales competitive with charge carrier lifetimes. These insights demonstrate that static charge transport networks are qualitatively inadequate, whereas average networks often overestimate network connectivity. Finally, a simple methodology for tracking dynamic charge transport properties is proposed.},
doi = {10.1073/pnas.1601915113},
url = {https://www.osti.gov/biblio/1267525}, journal = {Proceedings of the National Academy of Sciences of the United States of America},
issn = {0027-8424},
number = 31,
volume = 113,
place = {United States},
year = {2016},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at https://doi.org/10.1073/pnas.1601915113

Citation Metrics:
Cited by: 3 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Mesoscale molecular network formation in amorphous organic materials
journal, June 2014


Perylene diimides based materials for organic solar cells
journal, July 2013


Efficient Band Gap Prediction for Solids
journal, November 2010


Development and Testing of the OPLS All-Atom Force Field on Conformational Energetics and Properties of Organic Liquids
journal, January 1996


Steering Electrons on Moving Pathways
journal, October 2009


Charge Transport in Self-Assembled Semiconducting Organic Layers: Role of Dynamic and Static Disorder
journal, May 2010


Charge Transport in Disordered Organic Photoconductors a Monte Carlo Simulation Study
journal, January 1993


A multiscale description of charge transport in conjugated oligomers
journal, April 2010


Dynamics of the Excitonic Coupling in Organic Crystals
journal, January 2015


The Transient Localization Scenario for Charge Transport in Crystalline Organic Materials
journal, January 2016


Charge Transport in Organic Semiconductors
journal, April 2007


Dynamics of the Intermolecular Transfer Integral in Crystalline Organic Semiconductors
journal, March 2006


Modeling Charge Transport in Organic Photovoltaic Materials
journal, November 2009


Theoretical Characterization of the Structural and Hole Transport Dynamics in Liquid-Crystalline Phthalocyanine Stacks
journal, October 2009


Reducing dynamic disorder in small-molecule organic semiconductors by suppressing large-amplitude thermal motions
journal, February 2016


A Simple Index for Characterizing Charge Transport in Molecular Materials
journal, March 2015


Self-energy operators and exchange-correlation potentials in semiconductors
journal, June 1988


The Spectral Signatures of Frenkel Polarons in H- and J-Aggregates
journal, March 2010


Substantial photovoltaic response and morphology tuning in benzo[1,2-b:6,5-b′]dithiophene (bBDT) molecular donors
journal, January 2014


A dynamical monte carlo algorithm for master equations with time-dependent transition rates
journal, November 1997


Microscopic Simulations of Charge Transport in Disordered Organic Semiconductors
journal, August 2011


Charge Transport in Organic Crystals: Role of Disorder and Topological Connectivity
journal, August 2010


Stochastic modeling of molecular charge transport networks
journal, November 2012


Perylene-3,4,9,10-tetracarboxylic Acid Diimides: Synthesis, Physical Properties, and Use in Organic Electronics
journal, April 2011


Charge transport in high mobility molecular semiconductors: classical models and new theories
journal, January 2011


Contemporary Issues in Electron Transfer Research
journal, January 1996


    Works referencing / citing this record:

    Charge Transfer and Interface Effects in Co‐Assembled Circular Donor/Acceptor Complexes for Organic Photovoltaics
    journal, February 2019


    Molecular Understanding of Fullerene - Electron Donor Interactions in Organic Solar Cells
    journal, September 2016


    Unexpectedly Large Couplings Between Orthogonal Units in Anthraquinone Polymers
    journal, October 2019


    A map of high-mobility molecular semiconductors
    journal, September 2017


    New frontiers for the materials genome initiative
    journal, April 2019


    On the importance of detailed structure in molecular electronics (and why microscopic models cannot see the wood for trees)
    journal, September 2018