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

Preston, Riley J., Kershaw, Vincent F., and Kosov, Daniel S. (2020) Current-induced atomic motion, structural instabilities, and negative temperatures on molecule-electrode interfaces in electronic junctions. Physical Review B, 101. 155415.

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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 timescales 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.

Item ID: 63115
Item Type: Article (Research - C1)
ISSN: 2469-9969
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Copyright Information: © 2020 American Physical Society
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A version of this publication was included as Chapter 4 of the following PhD thesis: Kershaw, Vincent Francis (2020) Non-adiabatic quantum transport and atomic motion in molecular-sized electronic systems. PhD thesis, James Cook University, which is available Open Access in ResearchOnline@JCU. Please see the Related URLs for access.

Date Deposited: 21 Jul 2020 23:38
FoR Codes: 51 PHYSICAL SCIENCES > 5104 Condensed matter physics > 510499 Condensed matter physics not elsewhere classified @ 100%
SEO Codes: 97 EXPANDING KNOWLEDGE > 970102 Expanding Knowledge in the Physical Sciences @ 100%
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