Spin-Flip Unitary Coupled Cluster Method: Toward Accurate Description of Strong Electron Correlation on Quantum Computers

TL;DR

This paper introduces a combined spin-flip and unitary coupled cluster method using quantum equation-of-motion to improve the simulation of strongly correlated electron systems on quantum computers, outperforming previous methods.

Contribution

It develops a novel qEOM-SF-UCCSD/VQE approach that enhances the accuracy of simulating strong electron correlation phenomena on quantum computers.

Findings

qEOM-SF-UCCSD/VQE accurately predicts barrier heights in ethylene and cyclobutadiene.

The method outperforms standard UCCSD/VQE in strongly correlated systems.

Predicted values align well with experimental data.

Abstract

Quantum computers have emerged as a promising platform to simulate the strong electron correlation that is crucial to catalysis and photochemistry. However, owing to the choice of a trial wave function employed in the popular hybrid quantum-classical variational quantum eigensolver (VQE) algorithm, the accurate simulation is restricted to certain classes of correlated phenomena. Herein, we combine the spin-flip (SF) formalism with the unitary coupled cluster with singles and doubles (UCCSD) method via the quantum equation-of-motion (qEOM) approach to allow for an efficient simulation of a large family of strongly correlated problems. In particular, we show that the developed qEOM-SF-UCCSD/VQE method outperforms its UCCSD/VQE counterpart for simulation of the cis-trans isomerization of ethylene and the automerization of cyclobutadiene. The predicted qEOM-SF-UCCSD/VQE barrier heights for these two problems are in a good agreement with the experimentally determined values. The methodological developments presented herein will further stimulate investigation of this approach for the simulation of other types of correlated/entangled phenomena on a quantum computer.