Transport gap renormalization at a metal-molecule interface using DFT-NEGF and spin unrestricted calculations

Gil, J.A.; Thijssen, Jos

doi:10.1063/1.4999469

Cited by 8 publications

(3 citation statements)

References 51 publications

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“…In this realm, a significant advancement was made in recent work by Celis Gil and Thijssen (2017). They determined the shift parameters for the scissors operators in a self-consistent procedure by computationally gating the molecule inside the junction and monitoring the evolution of charge with the gate voltage QðV g Þ.…”

Section: Discussion Of Kohn-sham Transport Calculationsmentioning

confidence: 99%

Advances and challenges in single-molecule electron transport

et al. 2020

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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.

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Section: Discussion Of Kohn-sham Transport Calculationsmentioning

confidence: 99%

Advances and challenges in single-molecule electron transport

et al. 2020

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“…Furthermore, it is important to note that, although the energy difference between the LS and HS states exceeds 0.5 eV, the FePc molecule, which is often placed on a conducting surface in experiments, may experience altered chemical potential. This can modify spin-related energy variations due to the screening effects of the substrate. ,, We also note that the calculations in Figure are for the isolated molecule in equilibrium, whereas in the nonequilibrium STM setup relevant for IETS, the symmetry of the electrode orbitals dictates the coupling to certain Fe 3d orbitals, as seen already in the elastic transport calculations in Figure . The image charge and nonequilibrium inelastic effects will be pursued in future work.…”

mentioning

confidence: 73%

“…This can modify spin-related energy variations due to the screening effects of the substrate. 34,40,41 We also note that the calculations in Figure 5 are for the isolated molecule in equilibrium, whereas in the nonequilibrium STM setup relevant for IETS, the symmetry of the electrode orbitals dictates the coupling to certain Fe 3d orbitals, as seen already in the elastic transport calculations in Figure 1. The image charge and nonequilibrium inelastic effects will be pursued in future work.…”

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confidence: 75%

Strong Electron-Vibration Signals in Weakly Coupled Molecular Junctions: Activation of Spin-Crossover

Zhang,

Giménez-Santamarina,

Cardona-Serra

et al. 2024

Nano Lett.

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Manipulating individual molecular spin states with electronic current has the potential to revolutionize quantum information devices. However, it is still unclear how a current can cause a spin transition in single-molecule devices. Here, we propose a spin-crossover (SCO) mechanism induced by electron−phonon coupling in an iron(II) phthalocyanine molecule situated on a graphene-decoupled Ir(111) substrate. We performed simulations of both elastic and inelastic electron tunneling spectroscopy (IETS), which reveal current-induced Fe−N vibrations and an underestimation of established electron-vibration signals. Going beyond standard perturbation theory, we examined molecules in various charge and spin states using the Franck−Condon framework. The increased probability of spin switching suggests that notable IETS signals indicate SCO triggered by the inelastic vibrational excitation associated with Fe−N stretching.

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