Basis Set Generation and Optimization in the NISQ Era with Quiqbox.jl.

Abstract

In the noisy intermediate-scale quantum era, ab initio computation of electronic structure problems has become one of the major benchmarks for identifying the boundary between classical and quantum computational power. Basis sets play a key role in the electronic structure methods implemented on both classical and quantum devices. To investigate the consequences of single-particle basis sets, we propose a framework for more customizable basis set generation and optimization. This framework allows composite basis sets to go beyond typical basis set frameworks, such as atomic basis sets, by introducing the concept of mixed-contracted Gaussian-type orbitals. These basis set generations set the stage for more flexible variational optimization of basis set parameters. To realize this framework, we have developed an open-source software package named "Quiqbox" in the Julia programming language. We demonstrate various examples of using Quiqbox for basis set optimization and generation, ranging from optimizing atomic basis sets on the Hartree-Fock level, preparing the initial state for variational quantum eigensolver computation, and constructing basis sets with completely delocalized orbitals. We also include various benchmarks of Quiqbox for basis set optimization and ab initial electronic structure computation.