Rapid Initial-State Preparation for the Quantum Simulation of Strongly Correlated Molecules

Abstract

Studies on quantum algorithms for ground-state energy estimation often assume perfect ground-state preparation; however, in reality the initial state will have imperfect overlap with the true ground state. Here, we address that problem in two ways: by faster preparation of matrix-product-state (MPS) approximations and by more efficient filtering of the prepared state to find the ground-state energy. We show how to achieve unitary synthesis with a Toffoli complexity about 7× lower than that in prior work and use that to derive a more efficient MPS-preparation method. For filtering, we present two different approaches: sampling and binary search. For both, we use the theory of window functions to avoid large phase errors and minimize the complexity. We find that the binary-search approach provides better scaling with the overlap at the cost of a larger constant factor, such that it will be preferred for overlaps less than about 0.003. Finally, we estimate the total resources to perform ground-state energy estimation of Fe-S cluster systems, including the FeMo cofactor by estimating the overlap of different MPS initial states with potential ground states of the FeMo cofactor using an extrapolation procedure. With a modest MPS bond dimension of 4000, our procedure produces an estimate of approximately 0.9 overlap squared with a candidate ground state of the FeMo cofactor, producing a total resource estimate of 7.3×1010 Toffoli gates; neglecting the search over candidates and assuming the accuracy of the extrapolation, this validates prior estimates that have used perfect ground-state overlap. This presents an example of a practical path to prepare states of high overlap in a challenging-to-compute chemical system. Published by the American Physical Society 2025