Deep-Neural-Network Solution of the Electronic Schrödinger Equation

September, 2020


The electronic Schrödinger equation describes fundamental properties of molecules and materials, but can only be solved analytically for the hydrogen atom. The numerically exact full configuration-interaction method is exponentially expensive in the number of electrons. Quantum Monte Carlo is a possible way out: it scales well to large molecules, can be parallelized, and its accuracy has, as yet, only been limited by the flexibility of the used wave function ansatz. Here we propose PauliNet, a deep-learning wave function ansatz that achieves nearly exact solutions of the electronic Schrödinger equation. PauliNet has a multireference Hartree-Fock solution built in as a baseline, incorporates the physics of valid wave functions, and is trained using variational quantum Monte Carlo (VMC). PauliNet outperforms comparable state-of-the-art VMC ansatzes for atoms, diatomic molecules and a strongly-correlated hydrogen chain by a margin and is yet computationally efficient. We anticipate that thanks to the favourable scaling with system size, this method may become a new leading method for highly accurate electronic-strucutre calculations on medium-sized molecular systems.

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