Neural network backflow for ab-initio quantum chemistry (2403.03286v2)

Abstract: The ground state of second-quantized quantum chemistry Hamiltonians provides access to an important set of chemical properties. Wavefunctions based on ML architectures have shown promise in approximating these ground states in a variety of physical systems. In this work, we show how to achieve state-of-the-art energies for molecular Hamiltonians using the the neural network backflow wave-function. To accomplish this, we optimize this ansatz with a variant of the deterministic optimization scheme based on SCI introduced by [Li, et. al JCTC (2023)] which we find works better than standard MCMC sampling. For the molecules we studied, NNBF gives lower energy states than both CCSD and other neural network quantum states. We systematically explore the role of network size as well as optimization parameters in improving the energy. We find that while the number of hidden layers and determinants play a minor role in improving the energy, there is significant improvements in the energy from increasing the number of hidden units as well as the batch size used in optimization with the batch size playing a more important role.