Efficient classical simulation of large-scale unitary cluster Jastrow circuits

Abstract

Recent experiments on quantum computers have challenged the limits of classical computation in chemistry, simulating ground states of strongly correlated molecules. Many of these experiments have utilized the unitary cluster Jastrow ansatz, a quantum circuit inspired by the unitary coupled cluster ansatz that can be tailored to current quantum hardware. Notably, the largest experiment in Sci. Adv. 11, 25 (2025) executed a quantum circuit with 77 qubits and 10,570 gates on an IBM quantum computer and performed classical post-processing with up to 6400 nodes on Fugaku to compute ground state energies better than Hartree-Fock. In this work, we present a polynomial time classical algorithm to compute the energy of any single-layer unitary cluster Jastrow circuit, independent of locality constraints for quantum hardware. Our algorithm can reproduce the largest experiment from Sci. Adv. 11, 25 (2025) in less than a minute on a laptop, and through circuit optimization enabled by fast simulation we achieve a lower ground state energy than the experiment.