Current-induced atomic motion, structural instabilities, and negative temperatures on molecule-electrode interfaces in electronic junctions

Abstract

Molecule-electrode interfaces in molecular electronic junctions are prone to chemical reactions, structural changes, and localized heating effects caused by electric current. These can be exploited for device functionality or may be degrading processes that limit performance and device lifetime. We develop a nonequilibrium Green's function based transport theory in which the central region atoms and, more importantly, atoms on molecule-electrode interfaces are allowed to move. The separation of time-scales of slow nuclear motion and fast electronic dynamics enables the algebraic solution of the Kadanoff-Baym equations in the Wigner space. As a result, analytical expressions for dynamical corrections to the adiabatically computed Green's functions are produced. These dynamical corrections depend not only on the instantaneous molecular geometry but also on the nuclear velocities. To make the theoretical approach fully self-consistent, the same time-separation approach is used to develop expressions for the adiabatic, dissipative, and stochastic components of current-induced forces in terms of adiabatic Green's functions. Using these current induced forces, the equation of motion for the nuclear degrees of freedom is cast in the form of a Langevin equation. The theory is applied to model molecular electronic junctions. We observe that the interplay between the value of the spring constant for the molecule-electrode chemical bond and electronic coupling strength to the corresponding electrode is critical for the appearance of structural instabilities and, consequently, telegraphic switching in the electric current. The range of model parameters is identified to observe structurally stable molecular junctions as well as various different kinds of current-induced telegraphic switching. The interfacial structural instabilities are also quantified based on current noise calculations.

References in corpus (55)

• Molecular Transport Junctions: Vibrational Effects
• Franck-Condon blockade and giant Fano factors in transport through single molecules
• Phonon effects in molecular transistors: Quantum and classical treatment
• Nanomechanical Resonators and Their Applications in Biological/Chemical Detection: Nanomechanics Principles
• Inelastic transport theory from first-principles: methodology and applications for nanoscale devices
• Resonant inelastic tunneling in molecular junctions
• Resonant Electron Transport in Single-Molecule Junctions: Vibrational Excitation, Rectification, Negative Differential Resistance and Local Cooling
• Resonant electron heating and molecular phonon cooling in single C${}_{60}$ junctions
• Hierarchical Quantum Master Equation Approach to Electronic-Vibrational Coupling in Nonequilibrium Transport through Nanosystems
• Scattering theory of current-induced forces in mesoscopic systems
• Current-induced forces in mesoscopic systems: a scattering matrix approach
• Current-induced atomic dynamics, instabilities, and Raman signals: Quasi-classical Langevin equation approach
• Born-Oppenheimer Dynamics, Electronic Friction, and the Inclusion of Electron-Electron Interactions
• Full counting statistics of vibrationally-assisted electronic conduction: transport and fluctuations of the thermoelectric efficiency
• Nonequilibrium quantum systems with electron-phonon interactions: Transient dynamics and approach to steady state
• Inelastic tunneling effects on noise properties of molecular junctions
• Self-consistent theory of molecular switching
• Multimode vibrational effects in single molecule conductance: A nonequilibrium Green's function approach
• Resonant vibrations, peak broadening and noise in single molecule contacts: beyond the resonant tunnelling picture
• Scattering theory of adiabatic reaction forces due to out-of-equilibrium quantum environments
• Laser-like vibrational instability in rectifying molecular conductors
• Current-induced bond rupture in single-molecule junctions
• Shot noise suppression at room temperature in atomic-scale Au junctions
• Current-induced forces and hot-spots in biased nano-junctions
• Out-of-equilibrium catalysis of chemical reactions by electronic tunnel currents
• Kramers problem for nonequilibrium current-induced chemical reactions
• Current Noise in Single-Molecule Junctions Induced by Electronic-Vibrational Coupling
• Electronic friction near metal surfaces: a case where molecule-metal couplings depend on nuclear coordinates
• Effect of nonadiabatic electronic-vibrational interactions on the transport properties of single-molecule junctions
• Nonequilibrium resonant spectroscopy of molecular vibrons
• Current-induced forces for nonadiabatic molecular dynamics
• Signatures of the Current Blockade Instability in Suspended Carbon Nanotubes
• The universality of electronic friction II: Equivalence of the quantum-classical Liouville equation approach with von Oppen's nonequilibrium Green's function methods out of equilibrium
• Euler buckling instability and enhanced current blockade in suspended single-electron transistors
• Waiting time distribution for electron transport in a molecular junction with electron-vibration interaction
• Molecular junctions and molecular motors: Including Coulomb repulsion in electronic friction using nonequilibrium Green's functions
• Nuclear dynamics at molecule-metal interfaces: A pseudoparticle perspective
• Discontinuous Euler instability in nanoelectromechanical systems
• Hierarchical quantum master equation approach to vibronic reaction dynamics at metal surfaces
• Adiabaticity in semiclassical nanoelectromechanical systems
• Superoperator coupled cluster method for nonequilibrium density matrix
• Nonequilibrium configuration interaction method for transport in correlated quantum systems
• Scattering approach to backaction in coherent nanoelectromechanical systems
• Non-renewal statistics for electron transport in a molecular junction with electron-vibration interaction
• Temporal evolution of resonant transmission under telegraph noise
• Electro-Mechanical Transition in Quantum dots
• Electronic friction in interacting systems
• Nonequilibrium Green's function theory for nonadiabatic effects in quantum electron transport
• Bistability and Displacement Fluctuations in a Quantum Nano-mechanical Oscillator
• Large current noise in nanoelectromechanical systems close to continuous mechanical instabilities
• Non-equilibrium Green's function theory for non-adiabatic effects in quantum transport: inclusion of electron-electron interactions
• Telegraph noise in Markovian master equation for electron transport through molecular junctions
• Non-adiabatic dynamics of electrons and atoms under non-equilibrium conditions
• Nonadiabatic corrections to electric current in molecular junction due to nuclear motion at the molecule-electrode interfaces
• Fluctuating-time and full counting statistics for quantum transport in a system with internal telegraphic noise

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• Nonequilibrium reaction rate theory: Formulation and implementation within the hierarchical equations of motion approach
• First-passage time theory of activated rate chemical processes in electronic molecular junctions
• Non-Adiabatic Effects of Nuclear Motion in Quantum Transport of Electrons: A Self-Consistent Keldysh-Langevin Study
• Current-induced bond rupture in single-molecule junctions: Effects of multiple electronic states and vibrational modes
• Cooling molecular electronic junctions by AC current
• Quantum transport in driven systems with vibrations: Floquet nonequilibrium Green's functions and the GD approximation
• Emergence of negative viscosities and colored noise under current-driven Ehrenfest molecular dynamics
• A physically realizable molecular motor driven by the Landauer blowtorch effect
• Current-induced one-dimensional diffusion of Co ad-atoms on graphene nanoribbons
• A semiclassical nonequilibrium Green's Function approach to electron transport in systems exhibiting electron-phonon couplings