A contracted quantum
eigensolver (CQE) finds a solution to the
many-electron Schrödinger equation by solving its integration
(or contraction) to the two-electron space—a contracted Schrödinger
equation (CSE)—on a quantum computer. When applied to the anti-Hermitian
part of the CSE (ACSE), the CQE iterations optimize the wave function,
with respect to a general product ansatz of two-body exponential unitary
transformations that can exactly solve the Schrödinger equation.
In this work, we accelerate the convergence of the CQE and its wave
function ansatz via tools from classical optimization theory. By treating
the CQE algorithm as an optimization in a local parameter space, we
can apply quasi-second-order optimization techniques, such as quasi-Newton
approaches or nonlinear conjugate gradient approaches. Practically,
these algorithms result in superlinear convergence of the wave function
to a solution of the ACSE. Convergence acceleration is important because
it can both minimize the accumulation of noise on near-term intermediate-scale
quantum (NISQ) computers and achieve highly accurate solutions on
future fault-tolerant quantum devices. We demonstrate the algorithm,
as well as some heuristic implementations relevant for cost-reduction
considerations, comparisons with other common methods such as variational
quantum eigensolvers, and a Fermionic-encoding-free form of the CQE.