# Enabling ab initio geometry optimization of strongly correlated systems with transferable deep quantum Monte Carlo

arXiv: https://arxiv.org/abs/2603.25381 · HTML: https://mlsanity.com/paper/2603.25381/

## Key facts

- No citing papers in the map yet (data through 14 Oct 2026).
- Builds on 9 of its 55 references that are in the map.
- First posted on arXiv 26 Mar 2026.

## Builds on (most cited first, 9 of 9)

- [A Self-Attention Ansatz for Ab-initio Quantum Chemistry](https://mlsanity.com/paper/2211.13672/) (2022)
- [Ab-Initio Potential Energy Surfaces by Pairing GNNs with Neural Wave Functions](https://mlsanity.com/paper/2110.05064/) (2021)
- [Electronic excited states in deep variational Monte Carlo](https://mlsanity.com/paper/2203.09472/) (2022)
- [Sampling-free Inference for Ab-Initio Potential Energy Surface Networks](https://mlsanity.com/paper/2205.14962/) (2022)
- [Accurate Computation of Quantum Excited States with Neural Networks](https://mlsanity.com/paper/2308.16848/) (2023)
- [An ab initio foundation model of wavefunctions that accurately describes chemical bond breaking](https://mlsanity.com/paper/2506.19960/) (2025)
- [Variational Monte Carlo on a Budget -- Fine-tuning pre-trained Neural Wavefunctions](https://mlsanity.com/paper/2307.09337/) (2023)
- [Accurate Ab-initio Neural-network Solutions to Large-Scale Electronic Structure Problems](https://mlsanity.com/paper/2504.06087/) (2025)
- [Ab-initio simulation of excited-state potential energy surfaces with transferable deep quantum Monte Carlo](https://mlsanity.com/paper/2503.19847/) (2025)

## Abstract (arXiv)

A faithful description of chemical processes requires exploring extended regions of the molecular potential energy surface (PES), which remains challenging for strongly correlated systems. Transferable deep-learning variational Monte Carlo (VMC) offers a promising route by efficiently solving the electronic Schr"odinger equation jointly across molecular geometries at consistently high accuracy, yet its stochastic nature renders direct exploration of molecular configuration space nontrivial. Here, we present a framework for highly accurate ab initio exploration of PESs that combines transferable deep-learning VMC with a cost-effective estimation of energies, forces, and Hessians. By continuously sampling nuclear configurations during VMC optimization of electronic wave functions, we obtain transferable descriptions that achieve zero-shot chemical accuracy within chemically relevant distributions of molecular geometries. Throughout the subsequent characterization of molecular configuration space, the PES is evaluated only sparsely, with local approximations constructed by estimating VMC energies and forces at sampled geometries and aggregating the resulting noisy data using Gaussian process regression. Our method enables accurate and efficient exploration of complex PES landscapes, including structure relaxation, transition-state searches, and minimum-energy pathways, for both ground and excited states. This opens the door to studying bond breaking, formation, and large structural rearrangements in systems with pronounced multi-reference character.