Periodic plane-wave electronic structure calculations on quantum computers

Abstract A procedure for defining virtual spaces, and the periodic one-electron two-electron integrals, plane-wave second quantized Hamiltonians has been developed, it was validated using full configuration interaction (FCI) calculations, as well executions of variational quantum eigensolver (VQE) circuits on Quantinuum’s ion trap computers accessed through Microsoft’s Azure Quantum service. This work is an extension to systems a new class algorithms in which spaces were generated by optimizing orbitals from small pairwise CI Hamiltonians, we term correlation optimized with abbreviation COVOs. In this extension, integration first Brillouin zone automatically incorporated into integrals. With these procedures, have able derive containing only few orbitals, that capture significant amount correlation. The focus manuscript comparing simulations molecules calculated basis sets large unit cells at $$\Gamma$$ ? -point, including images, results aperiodic cells. approach promising, obtain good agreement between LiH molecule. Calculations performed Quantinuum H1-1 computer produced surprisingly energies, error mitigation played role hardware calculations (noisy) simulator results. Using modest number circuit runs (500 shots), reproduced FCI values 1 COVO Hamiltonian 11 milliHartree, expected improve larger runs.