Systematic generation of finite-range atomic basis sets for linear-scaling calculations

TL;DR

This paper introduces a variational method for generating atomic basis sets with controlled range, improving efficiency and performance in linear-scaling density functional calculations.

Contribution

A new variational approach to optimize atomic orbitals with a single parameter, enhancing efficiency and scalability for density functional theory computations.

Findings

Comparable quality to existing schemes

Better performance in linear-scaling calculations

Effective control of basis set range

Abstract

Basis sets of atomic orbitals are very efficient for density functional calculations but lack a systematic variational convergence. We present a variational method to optimize numerical atomic orbitals using a single parameter to control their range. The efficiency of the basis generation scheme is tested and compared with other schemes for multiple zeta basis sets. The scheme shows to be comparable in quality to other widely used schemes albeit offering better performance for linear-scaling computations.