Sergey Chulkov | Searcharxiv

arXiv2024

Enabling Ab-Initio Molecular Dynamics under Bias: The CP2K+SMEAGOL Interface for Integrating Density Functional Theory and Non-Equilibrium Green Functions

Density functional theory (DFT) combined with non-equilibrium Greens functions (NEGF) is a powerful approach to model quantum transport under external bias potentials, at reasonable computational cost. In this work we present a new interface between the popular mixed Gaussian/plane wave electronic structure package CP2K and the NEGF code SMEAGOL, the most feature-rich implementation of DFT-NEGF available for CP2K to-date. The CP2K+SMEAGOL interface includes the implementation of current induced forces. We verify this implementation for a variety of systems: an infinite 1D Au wire, a parallel-plate capacitor and a Au-H2-Au junction. We find good agreement with SMEAGOL calculations performed with SIESTA for the same systems, and with the example of a solvated Au wire demonstrate for the first time that DFT-NEGF can be used to perform molecular dynamics simulations under bias of large-scale condensed phase systems under realistic operating conditions.

cond-mat.mtrl-sci↗

arXiv2020

CP2K: An Electronic Structure and Molecular Dynamics Software Package -- Quickstep: Efficient and Accurate Electronic Structure Calculations

CP2K is an open source electronic structure and molecular dynamics software package to perform atomistic simulations of solid-state, liquid, molecular and biological systems. It is especially aimed at massively-parallel and linear-scaling electronic structure methods and state-of-the-art ab-initio molecular dynamics simulations. Excellent performance for electronic structure calculations is achieved using novel algorithms implemented for modern high-performance computing systems. This review revisits the main capabilities of CP2k to perform efficient and accurate electronic structure simulations. The emphasis is put on density functional theory and multiple post-Hartree-Fock methods using the Gaussian and plane wave approach and its augmented all-electron extension.

physics.chem-ph↗