Faster and lower scaling orbital-space Variational Monte Carlo

TL;DR

This paper presents three algorithmic improvements to orbital-space variational Monte Carlo, significantly reducing computational cost and scaling, enabling efficient large-scale electronic structure calculations.

Contribution

The authors introduce integral screening, rejection-free CTMC sampling, and adaptive optimization to enhance VMC efficiency and scalability.

Findings

Achieved $O(N^{1.2})$ scaling for Hubbard model

Calculated ground state energy of 160 H atoms in 25 CPU hours

Reduced computational cost by several orders of magnitude

Abstract

In this work, we introduce three algorithmic improvements to reduce the cost and improve the scaling of orbital space variational Monte Carlo (VMC). First, we show that by appropriately screening the one- and two-electron integrals of the Hamiltonian one can improve the efficiency of the algorithm by several orders of magnitude. This improved efficiency comes with the added benefit that the resulting algorithm scales as the second power of the system size $O(N^2)$, down from the fourth power $O(N^4)$. Using numerical results, we demonstrate that the practical scaling obtained is in fact $O(N^{1.5})$ for a chain of Hydrogen atoms, and $O(N^{1.2})$ for the Hubbard model. Second, we introduce the use of the rejection-free continuous time Monte Carlo (CTMC) to sample the determinants. CTMC is usually prohibitively expensive because of the need to calculate a large number of intermediates. Here, we take advantage of the fact that these intermediates are already calculated during the evaluation of the local energy and consequently, just by storing them one can use the CTCM algorithm with virtually no overhead. Third, we show that by using the adaptive stochastic gradient descent algorithm called AMSGrad one can optimize the wavefunction energies robustly and efficiently. The combination of these three improvements allows us to calculate the ground state energy of a chain of 160 hydrogen atoms using a wavefunction containing $\sim 2\times 10^5$ variational parameters with an accuracy of 1 $mE_h$/particle at a cost of just 25 CPU hours, which when split over 2 nodes of 24 processors each amounts to only about half hour of wall time. This low cost coupled with embarrassing parallelizability of the VMC algorithm and great freedom in the forms of usable wavefunctions, represents a highly effective method for calculating the electronic structure of model and \emph{ab initio} systems.