Quantum Solvers for Plane-Wave Hamiltonians: Abridging Virtual Spaces Through the Optimization of Pairwise Correlations

For many-body methods such as MCSCF and CASSCF, in which the number of one-electron orbitals is optimized independent basis set used, there are no problems with using plane-wave sets. However, for currently used quantum computing select configuration interaction (CI) coupled cluster (CC) methods, it necessary to have a virtual space that able capture significant amount electron-electron correlation system. The pseudopotential Hartree–Fock calculation, because Coulomb repulsion, often scattering states interact very weakly filled orbitals. As result, little energy captured from them. use spaces derived operators has also been tried, while some correlations captured, quite low. To overcome these limitations, we developing new classes algorithms define by optimizing small pairwise CI Hamiltonians, term abbreviation COVOs. With procedures, derive spaces, containing only few orbitals, correlation. focus this manuscript on sets target full (FCI) quality results H 2 near-term computers. initial approach were promising. We obtain good agreement FCI/cc-pVTZ system just 4 both FCI simulations. COVOs suggests may be possible them other approaches, including Møller–Plesset perturbation theories, open up door calculations methods.