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We unravel the critical role of vibrational mode softening in single-molecule electronic devices at high bias. Our theoretical analysis is carried out with a minimal model for molecular junctions, with mode softening arising due to quadratic electron-vibration couplings, and by developing a mean-field approach. We discover that the negative sign of the quadratic electron-vibration coupling coefficient can realize at high voltage a sharp negative differential resistance (NDR) effect with a large peak-to-valley ratio. Calculated current-voltage characteristics, obtained based on ab initio parameters for a nitro-substituted oligo(phenylene ethynylene) junction, agree very well with measurements. Our results establish that vibrational mode softening is a crucial effect at high voltage, underlying NDR, a substantial diode effect, and the breakdown of current-carrying molecular junctions.
We have observed tunable negative differential resistance (NDR) in scanning tunneling spectroscopy measurements of a double layer of C60 molecules on a metallic surface. Using a simple model we show that the observed NDR behavior is explained by volt
We propose a very accurate computational scheme for the dynamics of a classical oscillator coupled to a molecular junction driven by a finite bias, including the finite mass effect. We focus on two minimal models for the molecular junction: Anderson-
Nonlinear electrical properties, such as negative differential resistance (NDR), are essential in numerous electrical circuits, including memristors. Several physical origins have been proposed to lead to the NDR phenomena in semiconductor devices in
Introduction (2) Experimental background: Test beds (8) Theoretical approaches: A microscopic model(10) The electron-phonon coupling(14)Time and energy scales(15) Theoretical methods(19)Numerical calculations(28) Incoherent vs. coherent transpo
We show that Joule heating causes current-controlled negative differential resistance (CC-NDR) in TiO2 by constructing an analytical model of the voltage-current V(I) characteristic based on polaronic transport for Ohms Law and Newtons Law of Cooling