Atomistic simulations of highly conductive molecular transport junctions under realistic conditions

William R. French; Christopher R. Iacovella; Ivan Rungger; Amaury Melo Souza; Stefano Sanvito; Peter T. Cummings

doi:10.1039/c3nr00459g

Atomistic simulations of highly conductive molecular transport junctions under realistic conditions

William R. French, Christopher R. Iacovella, Ivan Rungger, Amaury Melo Souza, Stefano Sanvito, Peter T. Cummings

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Abstract

We report state-of-the-art atomistic simulations combined with high-fidelity conductance calculations to probe structure-conductance relationships in Au-benzenedithiolate (BDT)-Au junctions under elongation. Our results demonstrate that large increases in conductance are associated with the formation of monatomic chains (MACs) of Au atoms directly connected to BDT. An analysis of the electronic structure of the simulated junctions reveals that enhancement in the s-like states in Au MACs causes the increases in conductance. Other structures also result in increased conductance but are too short-lived to be detected in experiment, while MACs remain stable for long simulation times. Examinations of thermally evolved junctions with and without MACs show negligible overlap between conductance histograms, indicating that the increase in conductance is related to this unique structural change and not thermal fluctuation. These results, which provide an excellent explanation for a recently observed anomalous experimental result [Bruot et al., Nat. Nanotechnol., 2012, 7, 35-40], should aid in the development of mechanically responsive molecular electronic devices. © 2013 The Royal Society of Chemistry.

Original language	English (US)
Pages (from-to)	3654
Journal	Nanoscale
Volume	5
Issue number	9
DOIs	https://doi.org/10.1039/c3nr00459g
State	Published - 2013
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: WRF acknowledges partial support from the U.S. Department ofEducation for a Graduate Assistance in Areas of National Need(GAANN) Fellowship under grant number P200A090323; WRF,CRI and PTC acknowledge partial support from the NationalScience Foundation through grant CBET-1028374. IR, AMS, andSS thank the King Abdullah University of Science and Technology(ACRAB project) for financial support. This researchused resources of the National Energy Research ScientificComputing Center (NERSC), which is supported by the Office ofScience of the U.S. Department of Energy under Contract no.DE-AC02-05CH11231; specifically, the conductance calculationswere performed on NERSC's Carver.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

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title = "Atomistic simulations of highly conductive molecular transport junctions under realistic conditions",

abstract = "We report state-of-the-art atomistic simulations combined with high-fidelity conductance calculations to probe structure-conductance relationships in Au-benzenedithiolate (BDT)-Au junctions under elongation. Our results demonstrate that large increases in conductance are associated with the formation of monatomic chains (MACs) of Au atoms directly connected to BDT. An analysis of the electronic structure of the simulated junctions reveals that enhancement in the s-like states in Au MACs causes the increases in conductance. Other structures also result in increased conductance but are too short-lived to be detected in experiment, while MACs remain stable for long simulation times. Examinations of thermally evolved junctions with and without MACs show negligible overlap between conductance histograms, indicating that the increase in conductance is related to this unique structural change and not thermal fluctuation. These results, which provide an excellent explanation for a recently observed anomalous experimental result [Bruot et al., Nat. Nanotechnol., 2012, 7, 35-40], should aid in the development of mechanically responsive molecular electronic devices. {\textcopyright} 2013 The Royal Society of Chemistry.",

author = "French, {William R.} and Iacovella, {Christopher R.} and Ivan Rungger and Souza, {Amaury Melo} and Stefano Sanvito and Cummings, {Peter T.}",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: WRF acknowledges partial support from the U.S. Department ofEducation for a Graduate Assistance in Areas of National Need(GAANN) Fellowship under grant number P200A090323; WRF,CRI and PTC acknowledge partial support from the NationalScience Foundation through grant CBET-1028374. IR, AMS, andSS thank the King Abdullah University of Science and Technology(ACRAB project) for financial support. This researchused resources of the National Energy Research ScientificComputing Center (NERSC), which is supported by the Office ofScience of the U.S. Department of Energy under Contract no.DE-AC02-05CH11231; specifically, the conductance calculationswere performed on NERSC's Carver. This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

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AU - French, William R.

AU - Iacovella, Christopher R.

AU - Rungger, Ivan

AU - Souza, Amaury Melo

AU - Sanvito, Stefano

AU - Cummings, Peter T.

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: WRF acknowledges partial support from the U.S. Department ofEducation for a Graduate Assistance in Areas of National Need(GAANN) Fellowship under grant number P200A090323; WRF,CRI and PTC acknowledge partial support from the NationalScience Foundation through grant CBET-1028374. IR, AMS, andSS thank the King Abdullah University of Science and Technology(ACRAB project) for financial support. This researchused resources of the National Energy Research ScientificComputing Center (NERSC), which is supported by the Office ofScience of the U.S. Department of Energy under Contract no.DE-AC02-05CH11231; specifically, the conductance calculationswere performed on NERSC's Carver. This publication acknowledges KAUST support, but has no KAUST affiliated authors.

PY - 2013

Y1 - 2013

N2 - We report state-of-the-art atomistic simulations combined with high-fidelity conductance calculations to probe structure-conductance relationships in Au-benzenedithiolate (BDT)-Au junctions under elongation. Our results demonstrate that large increases in conductance are associated with the formation of monatomic chains (MACs) of Au atoms directly connected to BDT. An analysis of the electronic structure of the simulated junctions reveals that enhancement in the s-like states in Au MACs causes the increases in conductance. Other structures also result in increased conductance but are too short-lived to be detected in experiment, while MACs remain stable for long simulation times. Examinations of thermally evolved junctions with and without MACs show negligible overlap between conductance histograms, indicating that the increase in conductance is related to this unique structural change and not thermal fluctuation. These results, which provide an excellent explanation for a recently observed anomalous experimental result [Bruot et al., Nat. Nanotechnol., 2012, 7, 35-40], should aid in the development of mechanically responsive molecular electronic devices. © 2013 The Royal Society of Chemistry.

AB - We report state-of-the-art atomistic simulations combined with high-fidelity conductance calculations to probe structure-conductance relationships in Au-benzenedithiolate (BDT)-Au junctions under elongation. Our results demonstrate that large increases in conductance are associated with the formation of monatomic chains (MACs) of Au atoms directly connected to BDT. An analysis of the electronic structure of the simulated junctions reveals that enhancement in the s-like states in Au MACs causes the increases in conductance. Other structures also result in increased conductance but are too short-lived to be detected in experiment, while MACs remain stable for long simulation times. Examinations of thermally evolved junctions with and without MACs show negligible overlap between conductance histograms, indicating that the increase in conductance is related to this unique structural change and not thermal fluctuation. These results, which provide an excellent explanation for a recently observed anomalous experimental result [Bruot et al., Nat. Nanotechnol., 2012, 7, 35-40], should aid in the development of mechanically responsive molecular electronic devices. © 2013 The Royal Society of Chemistry.

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DO - 10.1039/c3nr00459g

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SN - 2040-3364

VL - 5

SP - 3654

JO - Nanoscale

JF - Nanoscale

IS - 9

ER -

Atomistic simulations of highly conductive molecular transport junctions under realistic conditions

Abstract

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