Large-Scale Atomistic Simulations of Environmental Effects on the Formation and Properties of Molecular Junctions

Abstract

Using an updated simulation tool, we examine molecular junctions comprised of benzene-1,4-dithiolate bonded between gold nanotips, focusing on the importance of environmental factors and inter-electrode distance on the formation and structure of bridged molecules. We investigate the complex relationship between monolayer density and tip separation, finding that the formation of multi-molecule junctions is favored at low monolayer density, while single-molecule junctions are favored at high density. We demonstrate that tip geometry and monolayer interactions, two factors that are often neglected in simulation, affect the bonding geometry and tilt angle of bridged molecules. We further show that the structures of bridged molecules at 298 and 77 K are similar.

arXiv commentTo appear in ACS Nano, 30 pages, 5 figures

References in corpus (9)

• Dependence of Single Molecule Junction Conductance on Molecular Conformation
• Single-Molecule Circuits with Well-Defined Molecular Conductance
• Charge Transport in Single Au|Alkanedithiol|Au Junctions: Coordination Geometries and Conformational Degrees of Freedom
• Efficient atomic self-interaction correction scheme for non-equilibrium quantum transport
• Effects of gating and contact geometry on current through conjugated molecules covalently bonded to electrodes
• Massively parallel computing on an organic molecular layer
• The Influence of Molecular Adsorption on Elongating Gold Nanowires
• The Role of Polytetrahedral Structures in the Elongation and Rupture of Gold Nanowires
• Influence of structural disorder and large-scale geometric fluctuations on the Coherent Transport of Metallic Junctions and Molecular Wires

Cited by in corpus (5)

• Adsorption-Induced Solvent-Based Electrostatic Gating of Charge Transport through Molecular Junctions
• Atomistic Simulations of Highly Conductive Molecular Transport Junctions Under Realistic Conditions
• Structural Origins of Conductance Fluctuations in Gold-Thiolate Molecular Transport Junctions
• Microscopic Theory, Analysis, and Interpretation of Conductance Histograms in Molecular Junctions
• Probing the Statistical Validity of the Ductile-to-Brittle Transition in Metallic Nanowires Using GPU Computing