Chemical accuracy from small, system-adapted basis functions

Abstract

We propose a general method for constructing system-dependent basis functions for correlated quantum chemical calculations. Our construction combines features from several traditional approaches: plane waves, localized basis functions, and wavelets. In a one-dimensional mimic of Coulomb systems, it requires only 2-3 basis functions per electron to achieve chemical accuracy, and reproduces the natural orbitals. We illustrate its effectiveness for molecular energy curves and chains of many atoms. We discuss the promise and challenges for realistic quantum chemical calculations.

14 pages, 12 figures, 2 tables, 102 references

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Cited by in corpus (6)

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• Continuous matrix product states for non-relativistic quantum fields: a lattice algorithm for inhomogeneous systems
• Density functionals and Kohn-Sham potentials with minimal wavefunction preparations on a quantum computer
• Conditional probability density functional theory
• Build your own tensor network library: DMRjulia I. Basic library for the density matrix renormalization group
• Bundled matrix product states represent low-energy excitations faithfully