Precise Quantum Chemistry calculations with few Slater Determinants

• URL: http://arxiv.org/abs/2503.14502v2
• Date: Fri, 02 May 2025 09:43:15 GMT
• Title: Precise Quantum Chemistry calculations with few Slater Determinants
• Authors: Clemens Giuliani, Jannes Nys, Rocco Martinazzo, Giuseppe Carleo, Riccardo Rossi,
• Abstract summary: Slater determinants have underpinned quantum chemistry for nearly a century, yet their full potential has remained challenging to exploit.<n>We show that a variational wavefunction composed of a few hundred optimized non-orthogonal determinants can achieve energy accuracies comparable to the state of the art.
• Score: 0.0
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: Slater determinants have underpinned quantum chemistry for nearly a century, yet their full potential has remained challenging to exploit. In this work, we show that a variational wavefunction composed of a few hundred optimized non-orthogonal determinants can achieve energy accuracies comparable to the state of the art. This is obtained by introducing an optimization method that leverages the quadratic dependence of the variational energy on the orbitals of each determinant, enabling an exact iterative optimization, and uses an efficient tensor-contraction algorithm to evaluate the effective Hamiltonian with a computational cost that scales as the fourth power of the number of basis functions. We benchmark the accuracy of the proposed method with exact full-configuration interaction results where available, and we achieve lower variational energies than coupled cluster (CCSD(T)) for several molecules in the double-zeta basis.

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