Multi-space excitation as an alternative to the Landauer picture for non-equilibrium quantum transport

Abstract

While the Landauer viewpoint constitutes a modern basis to understand nanoscale electronic transport and to realize first-principles implementations of the non-equilibrium Green's function (NEGF) formalism, seeking an alternative picture could be beneficial for the fundamental understanding and practical calculations of quantum transport processes. Herein, introducing a micro-canonical picture that maps the finite-bias quantum transport process to a drain-to-source or multi-electrode optical excitation, the multi-space constrained-search density functional theory (MS-DFT) formalism for first-principles electronic structure and quantum transport calculations is developed. Performing MS-DFT calculations for the benzenedithiolate single-molecule junction, it is shown that MS-DFT and standard DFT-NEGF calculations produce practically equivalent electronic and transmission data. Importantly, the variational convergence of "non-equilibrium total energy" within MS-DFT is demonstrated, which should have significant implications for in operando studies of nanoscale devices. Establishing a viable alternative to the Landauer viewpoint, the developed formalism should provide valuable atomistic information in the development of next-generation nanodevices.

arXiv comment9 pages, 3 figures

References in corpus (16)

• The SIESTA method for ab initio order-N materials simulation
• Efficient index handling of multidimensional periodic boundary conditions
• Density functional method for nonequilibrium electron transport
• Maximally localized Wannier functions: Theory and applications
• Improvements on non-equilibrium and transport Green function techniques: the next-generation transiesta
• Electron Transport Through Molecules: Self-consistent and Non-self-consistent Approaches
• Microscopic study of electrical transport through individual molecules with metallic contacts: II. Effect of the interface structure
• Efficient atomic self-interaction correction scheme for non-equilibrium quantum transport
• Contact Atomic Structure and Electron Transport Through Molecules
• Transport in nanoscale systems: the microcanonical versus grand-canonical picture
• Electrostatic potential profiles of molecular conductors
• Approach to steady state transport in nanoscale conductors
• Asymmetric I-V characteristics and magnetoresistance in magnetic point contacts
• Density-functional Study of Small Molecules within the Krieger-Li-Iafrate Approximation
• Stretching-induced conductance variations as fingerprints of contact configurations in single-molecule junctions
• Quasi-Fermi level splitting in nanoscale junctions from $\text{ab initio}$

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