Nonequilibrium Bond Forces in Single-Molecule Junctions

Jonathan Brand, Susanne Leitherer, Nick Rübner Papior, Nicolas Néel*, Yong Lei, Mads Brandbyge, Jörg Kröger

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Passing a current across two touching C60 molecules imposes a nonequilibrium population of bonding and antibonding molecular orbitals, which changes the equilibrium bond character and strength. A current-induced bond force therefore contributes to the total force at chemical-bond distances. The combination of first-principles calculations with scanning probe experiments exploring currents and forces in a wide C60-C60 distance range consistently evidences the presence of current-induced attraction that occurs when the two molecules are on the verge of forming a chemical bond. The unique opportunity to arrange matter at the atomic scale with the atomic force and scanning tunneling microscope tip has enabled closely matching molecular junctions in theory and experiment. The findings consequently represent the first report of current-induced bond forces at the single-molecule level and further elucidate the intimate relation between charge transport and force. The results are relevant to molecular electronics and chemical reactions in the presence of a current.
Original languageEnglish
JournalNano Letters
Volume19
Issue number11
Pages (from-to)7845-7851
Number of pages7
ISSN1530-6984
DOIs
Publication statusPublished - 2019

Keywords

  • Density functional theory
  • Nonequilibrium Green's function
  • Atomic force microscopy
  • Scanning tunelling microscopy
  • Single-module junction
  • C60

Cite this

Brand, Jonathan ; Leitherer, Susanne ; Papior, Nick Rübner ; Néel, Nicolas ; Lei, Yong ; Brandbyge, Mads ; Kröger, Jörg. / Nonequilibrium Bond Forces in Single-Molecule Junctions. In: Nano Letters. 2019 ; Vol. 19, No. 11. pp. 7845-7851.
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abstract = "Passing a current across two touching C60 molecules imposes a nonequilibrium population of bonding and antibonding molecular orbitals, which changes the equilibrium bond character and strength. A current-induced bond force therefore contributes to the total force at chemical-bond distances. The combination of first-principles calculations with scanning probe experiments exploring currents and forces in a wide C60-C60 distance range consistently evidences the presence of current-induced attraction that occurs when the two molecules are on the verge of forming a chemical bond. The unique opportunity to arrange matter at the atomic scale with the atomic force and scanning tunneling microscope tip has enabled closely matching molecular junctions in theory and experiment. The findings consequently represent the first report of current-induced bond forces at the single-molecule level and further elucidate the intimate relation between charge transport and force. The results are relevant to molecular electronics and chemical reactions in the presence of a current.",
keywords = "Density functional theory, Nonequilibrium Green's function, Atomic force microscopy, Scanning tunelling microscopy, Single-module junction, C60",
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doi = "10.1021/acs.nanolett.9b02845",
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Nonequilibrium Bond Forces in Single-Molecule Junctions. / Brand, Jonathan; Leitherer, Susanne; Papior, Nick Rübner; Néel, Nicolas; Lei, Yong; Brandbyge, Mads; Kröger, Jörg.

In: Nano Letters, Vol. 19, No. 11, 2019, p. 7845-7851.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Nonequilibrium Bond Forces in Single-Molecule Junctions

AU - Brand, Jonathan

AU - Leitherer, Susanne

AU - Papior, Nick Rübner

AU - Néel, Nicolas

AU - Lei, Yong

AU - Brandbyge, Mads

AU - Kröger, Jörg

PY - 2019

Y1 - 2019

N2 - Passing a current across two touching C60 molecules imposes a nonequilibrium population of bonding and antibonding molecular orbitals, which changes the equilibrium bond character and strength. A current-induced bond force therefore contributes to the total force at chemical-bond distances. The combination of first-principles calculations with scanning probe experiments exploring currents and forces in a wide C60-C60 distance range consistently evidences the presence of current-induced attraction that occurs when the two molecules are on the verge of forming a chemical bond. The unique opportunity to arrange matter at the atomic scale with the atomic force and scanning tunneling microscope tip has enabled closely matching molecular junctions in theory and experiment. The findings consequently represent the first report of current-induced bond forces at the single-molecule level and further elucidate the intimate relation between charge transport and force. The results are relevant to molecular electronics and chemical reactions in the presence of a current.

AB - Passing a current across two touching C60 molecules imposes a nonequilibrium population of bonding and antibonding molecular orbitals, which changes the equilibrium bond character and strength. A current-induced bond force therefore contributes to the total force at chemical-bond distances. The combination of first-principles calculations with scanning probe experiments exploring currents and forces in a wide C60-C60 distance range consistently evidences the presence of current-induced attraction that occurs when the two molecules are on the verge of forming a chemical bond. The unique opportunity to arrange matter at the atomic scale with the atomic force and scanning tunneling microscope tip has enabled closely matching molecular junctions in theory and experiment. The findings consequently represent the first report of current-induced bond forces at the single-molecule level and further elucidate the intimate relation between charge transport and force. The results are relevant to molecular electronics and chemical reactions in the presence of a current.

KW - Density functional theory

KW - Nonequilibrium Green's function

KW - Atomic force microscopy

KW - Scanning tunelling microscopy

KW - Single-module junction

KW - C60

U2 - 10.1021/acs.nanolett.9b02845

DO - 10.1021/acs.nanolett.9b02845

M3 - Journal article

VL - 19

SP - 7845

EP - 7851

JO - Nano Letters

JF - Nano Letters

SN - 1530-6984

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