Current-induced bond rupture in single-molecule junctions

Erpenbeck, A.; Schinabeck, C.; Peskin, Uri; Thoss, Michael

doi:10.1103/physrevb.97.235452

Cited by 48 publications

(71 citation statements)

References 115 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…In extreme cases, the current-induced forces can lead to bond rupture. Progress toward a better understanding of this phenomenon was made in recent work by Erpenbeck et al (2018).…”

Section: Discussion Of Nonlinearities In the I-v Characteristicsmentioning

confidence: 99%

Advances and challenges in single-molecule electron transport

et al. 2020

View full text Add to dashboard Cite

Electronic transport properties of single-molecule junctions have been widely measured by several techniques, including mechanically controllable break junctions, electromigration break junctions, and by means of scanning tunneling microscopes. In parallel, many theoretical tools have been developed and refined for describing such transport properties and for obtaining numerical predictions. Most prominent among these theoretical tools are those based upon density functional theory. In this review, theory and experiment are critically compared, and this confrontation leads to several important conclusions. The theoretically predicted trends nowadays reproduce the experimental findings well for series of molecules with a single well-defined control parameter, such as the length of the molecules. The quantitative agreement between theory and experiment usually is less convincing, however. Two main sources for the quantitative discrepancies can be identified. Experimentally, the atomic structure of the junction typically realized in the measurement is not well known, so simulations rely on plausible scenarios. In theory, correlation effects can be included only in approximations that are difficult to control for experimentally relevant situations. Therefore, one typically expects qualitative agreement with present modeling tools; in exceptional cases a quantitative agreement has already been achieved. For further progress, benchmark systems are required that are sufficiently well defined by experiment to allow quantitative testing of the approximation schemes underlying the theoretical modeling. Several key experiments can be identified suggesting that the present description may even be qualitatively incomplete in some cases. Such key experimental observations and their current models are also discussed here, leading to several suggestions for extensions of the models toward including dynamic image charges, electron correlations, and polaron formation.

show abstract

“…In extreme cases, the current-induced forces can lead to bond rupture. Progress toward a better understanding of this phenomenon was made in recent work by Erpenbeck et al (2018).…”

Section: Discussion Of Nonlinearities In the I-v Characteristicsmentioning

confidence: 99%

Advances and challenges in single-molecule electron transport

et al. 2020

View full text Add to dashboard Cite

show abstract

“…We recently used a similar model system to study current-induced dissociation in molecular junctions based on a mixed quantum classical methodology. [13] For a detailed presentation and discussion of the model and the potentials, we refer to Ref. 13.…”

Section: Resultsmentioning

confidence: 99%

Hierarchical quantum master equation approach to vibronic reaction dynamics at metal surfaces

Erpenbeck

Thoss

2019

The Journal of Chemical Physics

Self Cite

View full text Add to dashboard Cite

A novel quantum dynamical method to simulate vibronic reaction dynamics in molecules at metal surfaces is proposed. The method is based on the hierarchical quantum master equation approach and uses a discrete variable representation of the nuclear degrees of freedom in combination with complex absorbing potentials and an auxiliary source term. It provides numerically exact results for a range of models. By taking the coupling to the continuum of electronic states of the surface properly into account, nonadiabatic processes can be described and the effect of electronic friction is included in a nonperturbative and non-Markovian way. Illustrative application to models for desorption of a molecule at a surface and current-induced bond rupture in single-molecule junctions demonstrate the performance and versatility of the method.

show abstract

“…We have further demonstrated forces which exist without potential drop and can thus be considered as purely "current-induced". Our theoretical work can be help to understand current-induced strains, bond-breaking processes 34,35 , and mechanisms that lead to the destruction of devices at the atomic scale.…”

Section: Discussionmentioning

confidence: 99%

Current-induced atomic forces in gated graphene nanoconstrictions

2019

View full text Add to dashboard Cite

Electronic current densities can reach extreme values in highly conducting nanostructures where constrictions limit current. For bias voltages on the 1 volt scale, the highly non-equilibrium situation can influence the electronic density between atoms, leading to significant inter-atomic forces. An easy interpretation of the non-equilibrium forces is currently not available. In this work, we present an ab-initio study based on density functional theory of bias-induced atomic forces in gated graphene nanoconstrictions consisting of junctions between graphene electrodes and graphene nano-ribbons in the presence of current. We find that current-induced bond-forces and bond-charges are correlated, while bond-forces are not simply correlated to bond-currents. We discuss, in particular, how the forces are related to induced charges and the electrostatic potential profile (voltage drop) across the junctions. For long current-carrying junctions we may separate the junction into a part with a voltage drop, and a part without voltage drop. The latter situation can be compared to a nanoribbon in the presence of current using an ideal ballistic velocity-dependent occupation function. This shows how the combination of voltage drop and current give rise to the strongest currentinduced forces in nanostructures.

show abstract

Current-induced bond rupture in single-molecule junctions

Cited by 48 publications

References 115 publications

Advances and challenges in single-molecule electron transport

Advances and challenges in single-molecule electron transport

Hierarchical quantum master equation approach to vibronic reaction dynamics at metal surfaces

Current-induced atomic forces in gated graphene nanoconstrictions

Contact Info

Product

Resources

About