Efficient optimization of neural network backflow for <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>a</mml:mi> <mml:mi>b</mml:mi> </mml:mrow> <mml:mo> </mml:mo> <mml:mrow> <mml:mi>i</mml:mi> <mml:mi>n</mml:mi> <mml:mi>i

The ground state of second-quantized quantum chemistry Hamiltonians is key to determining molecular properties. Neural quantum states (NQSs) offer flexible and expressive wave-function Ans"atze for this task but face two main challenges: highly peaked ground-state wave functions hinder efficient sampling, and local energy evaluations scale quartically with system size, incurring significant computational costs. In this work, we overcome these challenges by introducing a suite of algorithmic enhancements, which includes efficient periodic compact subspace construction, truncated local energy evaluations, improved stochastic sampling, and physics-informed modifications. Applying these techniques to the neural network backflow Ansatz, we demonstrate significant gains in both accuracy and scalability. Our enhanced method surpasses traditional quantum chemistry methods like coupled cluster singles and doubles (CCSD) and CCSD and perturbative triples [CCSD(T)], outperforms other NQS approaches, and achieves competitive energies with state-of-the-art ab initio techniques such as heat-bath configuration interaction, adaptive sampling configuration interaction, full configuration interaction quantum Monte Carlo, and density matrix renormalization group. A series of ablation and comparative studies quantifies the contribution of each enhancement to the observed improvements in accuracy and efficiency. Furthermore, we investigate the representational capacity of the Ansatz, finding that its performance correlates with the inverse participation ratio, with more delocalized states being more challenging to approximate.

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Publication Details

Journal
Physical review. B./Physical review. B
Published
2025-09-23
DOI
https://doi.org/10.1103/thz7-lmdn
Citations
1
Primary Topic
Machine Learning in Materials Science
Type
article
Field-Weighted Citation Impact
0.52
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article

Efficient optimization of neural network backflow for <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>a</mml:mi> <mml:mi>b</mml:mi> </mml:mrow> <mml:mo> </mml:mo> <mml:mrow> <mml:mi>i</mml:mi> <mml:mi>n</mml:mi> <mml:mi>i

An-Jun Liu, Bryan K. Clark
1 citations
Physical review. B./Physical review. B
Machine Learning in Materials Science
0.52
article

Efficient optimization of neural network backflow for <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>a</mml:mi> <mml:mi>b</mml:mi> </mml:mrow> <mml:mo> </mml:mo> <mml:mrow> <mml:mi>i</mml:mi> <mml:mi>n</mml:mi> <mml:mi>i

An-Jun Liu, Bryan K. Clark
article en
1 citations

Abstract

The ground state of second-quantized quantum chemistry Hamiltonians is key to determining molecular properties. Neural quantum states (NQSs) offer flexible and expressive wave-function Ans\"atze for this task but face two main challenges: highly peaked ground-state wave functions hinder efficient sampling, and local energy evaluations scale quartically with system size, incurring significant computational costs. In this work, we overcome these challenges by introducing a suite of algorithmic enhancements, which includes efficient periodic compact subspace construction, truncated local energy evaluations, improved stochastic sampling, and physics-informed modifications. Applying these techniques to the neural network backflow Ansatz, we demonstrate significant gains in both accuracy and scalability. Our enhanced method surpasses traditional quantum chemistry methods like coupled cluster singles and doubles (CCSD) and CCSD and perturbative triples [CCSD(T)], outperforms other NQS approaches, and achieves competitive energies with state-of-the-art ab initio techniques such as heat-bath configuration interaction, adaptive sampling configuration interaction, full configuration interaction quantum Monte Carlo, and density matrix renormalization group. A series of ablation and comparative studies quantifies the contribution of each enhancement to the observed improvements in accuracy and efficiency. Furthermore, we investigate the representational capacity of the Ansatz, finding that its performance correlates with the inverse participation ratio, with more delocalized states being more challenging to approximate.

Physical review. B./Physical review. BVol. 112(15)
University of Illinois Urbana-Champaign (US)
Openalex Percentile: Top 31%
Machine Learning in Materials Science
0.52
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Efficient optimization of neural network backflow for <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>a</mml:mi> <mml:mi>b</mml:mi> </mml:mrow> <mml:mo> </mml:mo> <mml:mrow> <mml:mi>i</mml:mi> <mml:mi>n</mml:mi> <mml:mi>i — An-Jun Liu, Bryan K. Clark · Physical review. B./Physical review. B (2025) | TGRS Research Map | TGRS