Multi-sliced Gausslet Basis Sets for Electronic Structure

TL;DR

This paper presents a new highly local basis set for electronic structure calculations using gausslets, enabling more accurate correlation calculations near the complete basis set limit with efficient multislicing techniques.

Contribution

Introduction of multi-sliced gausslet basis sets that improve efficiency and accuracy in electronic structure calculations near the complete basis set limit.

Findings

Achieved errors near 0.1 mH per atom in hydrogen chains.

Enabled higher accuracy calculations with both Hartree Fock and DMRG methods.

Demonstrated efficiency of basis sets in correlation calculations.

Abstract

We introduce highly local basis sets for electronic structure which are very efficient for correlation calculations near the complete basis set limit. Our approach is based on gausslets, recently introduced wavelet-like smooth orthogonal functions. We adapt the gausslets to particular systems using one dimensional coordinate transformations, putting more basis functions near nuclei, while maintaining orthogonality. Three dimensional basis functions are composed out of products of the 1D functions in an efficient way called multislicing. We demonstrate the new bases with both Hartree Fock and density matrix renormalization group (DMRG) calculations on hydrogen chain systems. With both methods, we can go to higher accuracy in the complete basis set limit than is practical for conventional Gaussian basis sets, with errors near 0.1 mH per atom.