Structural Origins of Conductance Fluctuations in Gold–Thiolate Molecular Transport Junctions

Handle URI:
http://hdl.handle.net/10754/599757
Title:
Structural Origins of Conductance Fluctuations in Gold–Thiolate Molecular Transport Junctions
Authors:
French, William R.; Iacovella, Christopher R.; Rungger, Ivan; Souza, Amaury Melo; Sanvito, Stefano; Cummings, Peter T.
Abstract:
We report detailed atomistic simulations combined with high-fidelity conductance calculations to probe the structural origins of conductance fluctuations in thermally evolving Au-benzene-1,4-dithiolate-Au junctions. We compare the behavior of structurally ideal junctions (where the electrodes are modeled as flat surfaces) to structurally realistic, experimentally representative junctions resulting from break-junction simulations. The enhanced mobility of metal atoms in structurally realistic junctions results in significant changes to the magnitude and origin of the conductance fluctuations. Fluctuations are larger by a factor of 2-3 in realistic junctions compared to ideal junctions. Moreover, in junctions with highly deformed electrodes, the conductance fluctuations arise primarily from changes in the Au geometry, in contrast to results for junctions with nondeformed electrodes, where the conductance fluctuations are dominated by changes in the molecule geometry. These results provide important guidance to experimentalists developing strategies to control molecular conductance, and also to theoreticians invoking simplified structural models of junctions to predict their behavior. © 2013 American Chemical Society.
Citation:
French WR, Iacovella CR, Rungger I, Souza AM, Sanvito S, et al. (2013) Structural Origins of Conductance Fluctuations in Gold–Thiolate Molecular Transport Junctions. The Journal of Physical Chemistry Letters 4: 887–891. Available: http://dx.doi.org/10.1021/jz4001104.
Publisher:
American Chemical Society (ACS)
Journal:
The Journal of Physical Chemistry Letters
Issue Date:
21-Mar-2013
DOI:
10.1021/jz4001104
PubMed ID:
26291351
Type:
Article
ISSN:
1948-7185
Sponsors:
W.R.F. acknowledges partial support from the U.S. Department of Education for a Graduate Assistance in Areas of National Need (GAANN) Fellowship under Grant Number P200A090323; W.R.F., C.R.I., and P.T.C. acknowledge partial support from the National Science Foundation through Grant CBET-1028374. I.R., A.M.S., and S.S. thank the King Abdullah University of Science and Technology (ACRAB project) for financial support. This research used resources of the National Energy Research Scientific Computing Center (NERSC), which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231; specifically, the conductance calculations were performed on NERSC’s Carver.
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Full metadata record

DC FieldValue Language
dc.contributor.authorFrench, William R.en
dc.contributor.authorIacovella, Christopher R.en
dc.contributor.authorRungger, Ivanen
dc.contributor.authorSouza, Amaury Meloen
dc.contributor.authorSanvito, Stefanoen
dc.contributor.authorCummings, Peter T.en
dc.date.accessioned2016-02-28T06:09:06Zen
dc.date.available2016-02-28T06:09:06Zen
dc.date.issued2013-03-21en
dc.identifier.citationFrench WR, Iacovella CR, Rungger I, Souza AM, Sanvito S, et al. (2013) Structural Origins of Conductance Fluctuations in Gold–Thiolate Molecular Transport Junctions. The Journal of Physical Chemistry Letters 4: 887–891. Available: http://dx.doi.org/10.1021/jz4001104.en
dc.identifier.issn1948-7185en
dc.identifier.pmid26291351en
dc.identifier.doi10.1021/jz4001104en
dc.identifier.urihttp://hdl.handle.net/10754/599757en
dc.description.abstractWe report detailed atomistic simulations combined with high-fidelity conductance calculations to probe the structural origins of conductance fluctuations in thermally evolving Au-benzene-1,4-dithiolate-Au junctions. We compare the behavior of structurally ideal junctions (where the electrodes are modeled as flat surfaces) to structurally realistic, experimentally representative junctions resulting from break-junction simulations. The enhanced mobility of metal atoms in structurally realistic junctions results in significant changes to the magnitude and origin of the conductance fluctuations. Fluctuations are larger by a factor of 2-3 in realistic junctions compared to ideal junctions. Moreover, in junctions with highly deformed electrodes, the conductance fluctuations arise primarily from changes in the Au geometry, in contrast to results for junctions with nondeformed electrodes, where the conductance fluctuations are dominated by changes in the molecule geometry. These results provide important guidance to experimentalists developing strategies to control molecular conductance, and also to theoreticians invoking simplified structural models of junctions to predict their behavior. © 2013 American Chemical Society.en
dc.description.sponsorshipW.R.F. acknowledges partial support from the U.S. Department of Education for a Graduate Assistance in Areas of National Need (GAANN) Fellowship under Grant Number P200A090323; W.R.F., C.R.I., and P.T.C. acknowledge partial support from the National Science Foundation through Grant CBET-1028374. I.R., A.M.S., and S.S. thank the King Abdullah University of Science and Technology (ACRAB project) for financial support. This research used resources of the National Energy Research Scientific Computing Center (NERSC), which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231; specifically, the conductance calculations were performed on NERSC’s Carver.en
dc.publisherAmerican Chemical Society (ACS)en
dc.subjectbenzenedithiolen
dc.subjectconductance calculationsen
dc.subjectdensity functional theoryen
dc.subjectelectron transporten
dc.subjectgold nanowiresen
dc.subjectmolecular heterojunction electronicsen
dc.subjectmolecular simulationen
dc.subjectmolecular transport junctionsen
dc.titleStructural Origins of Conductance Fluctuations in Gold–Thiolate Molecular Transport Junctionsen
dc.typeArticleen
dc.identifier.journalThe Journal of Physical Chemistry Lettersen
dc.contributor.institutionVanderbilt University, Nashville, United Statesen
dc.contributor.institutionTrinity College Dublin, Dublin, Irelanden
dc.contributor.institutionOak Ridge National Laboratory, Oak Ridge, United Statesen

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