PyCDFT: A Python package for constrained density functional theory

TL;DR

PyCDFT is a flexible Python package that enables constrained density functional theory calculations for diabatic states, compatible with existing DFT codes, and validated through molecular dynamics and electronic coupling benchmarks.

Contribution

PyCDFT introduces an object-oriented, customizable Python implementation of CDFT that interfaces with DFT codes for accurate diabatic state computations.

Findings

PyCDFT produces results consistent with existing CDFT implementations.

It enables efficient calculations within a parallel molecular dynamics framework.

The package is robust and flexible for various CDFT applications.

Abstract

We present PyCDFT, a Python package to compute diabatic states using constrained density functional theory (CDFT). PyCDFT provides an object-oriented, customizable implementation of CDFT, and allows for both single-point self-consistent-field calculations and geometry optimizations. PyCDFT is designed to interface with existing density functional theory (DFT) codes to perform CDFT calculations where constraint potentials are added to the Kohn-Sham Hamiltonian. Here we demonstrate the use of PyCDFT by performing calculations with a massively parallel first-principles molecular dynamics code, Qbox, and we benchmark its accuracy by computing the electronic coupling between diabatic states for a set of organic molecules. We show that PyCDFT yields results in agreement with existing implementations and is a robust and flexible package for performing CDFT calculations. The program is available at https://github.com/hema-ted/pycdft/.