Resolving correlated states of benzyne with an error-mitigated contracted quantum eigensolver

Abstract

The simulation of strongly correlated many-electron systems is one of the most promising applications for near-term quantum devices. Here we use a class of eigenvalue solvers [presented in Smart and Mazziotti, Phys. Rev. Lett. 126, 070504 (2021)] in which a contraction of the Schr\"odinger equation is solved for the two-electron reduced density matrix (2-RDM) to resolve the energy splittings of the ortho-, meta-, and para-isomers of benzyne ${\text{C}}_{6}{\text{H}}_{4}$. In contrast to the traditional variational quantum eigensolver, the contracted quantum eigensolver can solve an integration (or contraction) of the many-electron Schr\"odinger equation onto the two-electron space. The quantum solution of the anti-Hermitian part of the contracted Schr\"odinger equation provides a scalable approach with few variational parameters that has its foundations in 2-RDM theory. Experimentally, a variety of error-mitigation strategies enable the calculation, including a linear shift in the 2-RDM targeting the iterative nature of the algorithm as well as a projection of the 2-RDM onto the convex set of approximately $N$-representable 2-RDMs defined by the 2-positive $N$-representability conditions. The relative energies exhibit single-digit millihartree errors, capturing a large part of the electron correlation energy, and the computed natural orbital occupations reflect the significant differences in the electron correlation of the isomers.

Topics & Concepts