Ab Initio Auxiliary-Field Quantum Monte Carlo in the Thermodynamic Limit

Ab initio auxiliary-field quantum Monte Carlo (AFQMC) is a systematically improvable many-body method, but its application to extended solids has been severely limited by unfavorable computational scaling and memory requirements that obstruct direct access to the thermodynamic and complete-basis-set limits. By combining tensor hypercontraction via interpolative separable density fitting with $\mathbf{k}$-point symmetry, we reduce the computational and memory scaling of ab initio AFQMC for solids to $O(N^3)$ and $O(N^2)$ with arbitrary basis, respectively, comparable to diffusion Monte Carlo. This enables direct and simultaneous thermodynamic-limit and complete-basis-set AFQMC calculations across insulating, metallic, and strongly correlated solids, without embedding, local approximations, empirical finite-size corrections, or composite schemes. Our results establish AFQMC as a general-purpose, systematically improvable alternative to diffusion Monte Carlo and coupled-cluster methods for predictive ab initio simulations of solids, enabling accurate energies and magnetic observables within a unified framework.

Source: arXiv:2602.16679v1 - http://arxiv.org/abs/2602.16679v1 PDF: https://arxiv.org/pdf/2602.16679v1 Original Link: http://arxiv.org/abs/2602.16679v1