Journal of Physical Chemistry Letters

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

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Quantum computers have emerged as a promising platform to simulate strong electron correlation that is crucial to catalysis and photochemistry. However, owing to the choice of a trial wave function employed in the variational quantum eigensolver (VQE) algorithm, 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. 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 and the predicted qEOM-SF-UCCSD/VQE barrier heights are in a good agreement with the experimentally determined values. The developments presented herein will further stimulate the investigation of this approach for simulations of other types of correlated/entangled phenomena on quantum computers.


28 Aug 2023


Journal of Physical Chemistry Letters