Automatic generation of input files with optimised k-point meshes for Quantum ESPRESSO self-consistent field single-point total energy calculations

Abstract

Performing density functional theory (DFT) calculations requires a careful choice of computational parameters to ensure convergence and obtain meaningful results. This represents a particularly important problem for high-throughput and agentic workflows, where due to computational cost, any additional convergence studies are preferably avoided. So, there is a need for tools and models which are able to predict DFT parameters from basic input information, such as a structure. In this work, we develop a machine learning approach to predict the appropriate k-point sampling in DFT calculations and generate the input files for Quantum Espresso self-consistent field calculations. To achieve this, we first generated a training dataset comprising over 20 000 materials, each with an energy convergence threshold of 1 meV per atom. Several ML models were evaluated for their ability to predict k-point distance, and uncertainty estimation was incorporated to guarantee that, for at least 85–95% of compounds, the predicted k-distance lies within the convergence region. The best-performing models are made publicly available through an open-access web application.