Journal article, 2012

The standard formulation of tunneling transport rests on an open-boundary modeling. There, conserving approximations to nonequilibrium Green function or quantum statistical mechanics provide consistent but computational costly approaches; alternatively, the use of density-dependent ballistic-transport calculations (e.g., Lang 1995 Phys. Rev. B 52 5335), here denoted 'DBT', provides computationally efficient (approximate) atomistic characterizations of the electron behavior but has until now lacked a formal justification. This paper presents an exact, variational nonequilibrium thermodynamic theory for fully interacting tunneling and provides a rigorous foundation for frozen-nuclei DBT calculations as a lowest-order approximation to an exact nonequilibrium thermodynamic density functional evaluation. The theory starts from the complete electron nonequilibrium quantum statistical mechanics and I identify the operator for the nonequilibrium Gibbs free energy which, generally, must be treated as an implicit solution of the fully interacting many-body dynamics. I demonstrate a minimal property of a functional for the nonequilibrium thermodynamic grand potential which thus uniquely identifies the solution as the exact nonequilibrium density matrix. I also show that the uniqueness-of-density proof from a closely related Lippmann-Schwinger collision density functional theory (Hyldgaard 2008 Phys. Rev. B 78 165109) makes it possible to express the variational nonequilibrium thermodynamic description as a single-particle formulation based on universal electron-density functionals; the full nonequilibrium single-particle formulation improves the DBT method, for example, by a more refined account of Gibbs free energy effects. I illustrate a formal evaluation of the zero-temperature thermodynamic grand potential value which I find is closely related to the variation in the scattering phase shifts and hence to Friedel density oscillations. This paper also discusses the difference between the here-presented exact thermodynamic forces and the often-used electrostatic forces. Finally the paper documents an inherent adiabatic nature of the thermodynamic forces and observes that these are suited for a nonequilibrium implementation of the Born-Oppenheimer approximation.

time-dependent

tight-binding

statistical-mechanics

linear-response theory

anderson impurity

transport

metal-surfaces

quantum transport

der-waals interactions

friedel sum rule

electron-phonon interaction

Chalmers, Applied Physics, Electronics Material and Systems Laboratory

0953-8984 (ISSN)

Vol. 24 42 Article Number: 424219 - 424219Nanoscience and Nanotechnology (2010-2017)

Materials Science

Physical Sciences

Other Physics Topics

Condensed Matter Physics

Basic sciences

10.1088/0953-8984/24/42/424219