Chemistry beyond the Hartree–Fock energy via quantum computed moments

Abstract

Abstract Quantum computers hold promise to circumvent the limitations of conventional computing for difficult molecular problems. However, the accumulation of quantum logic errors on real devices represents a major challenge, particularly in the pursuit of chemical accuracy requiring the inclusion of electronic correlation effects. In this work we implement the quantum computed moments (QCM) approach for hydrogen chain molecular systems up to H $$_6$$ 6 . On a superconducting quantum processor, Hamiltonian moments, $$\langle H^p\rangle$$ ⟨ H p ⟩ are computed with respect to the Hartree–Fock state, which are then employed in Lanczos expansion theory to determine an estimate for the ground-state energy which incorporates electronic correlations and manifestly improves on the direct energy measurement. Post-processing purification of the raw QCM data takes the estimate below the Hartree–Fock energy to within 99.9% of the exact electronic ground-state energy for the largest system studied, H $$_6$$ 6 . Calculated dissociation curves indicate precision at about 10mH for this system and as low as 0.1mH for molecular hydrogen, H $$_2$$ 2 , over a range of bond lengths. In the context of stringent precision requirements for chemical problems, these results provide strong evidence for the error suppression capability of the QCM method, particularly when coupled with post-processing error mitigation. While calculations based on the Hartree–Fock state are tractable to classical computation, these results represent a first step towards implementing the QCM method in a quantum chemical trial circuit. Greater emphasis on more efficient representations of the Hamiltonian and classical preprocessing steps may enable the solution of larger systems on near-term quantum processors.