Accuracy and Resource Estimations for Quantum Chemistry on a Near-term Quantum Computer.
The study and prediction of chemical reactivity is one of the most important application areas of molecular quantum chemistry. Large-scale, fully error-tolerant quantum computers could provide exact or near-exact solutions to the underlying electronic structure problem with exponentially less effort than a classical computer thus enabling highly accurate predictions for comparably large molecular systems. In the nearer future, however, only "noisy" devices with a limited number of qubits that are subject to decoherence will be available. For such near-term quantum computers the hybrid quantum-classical variational quantum eigensolver algorithm in combination with the unitary coupled-cluster ansatz (UCCSD-VQE) [Peruzzo, A.; McClean, J.; Shadbolt, P.; Yung, M.; Zhou, X.; Love, P.; Aspuru-Guzik, A.; O'Brien, J. L. Nature Comm. 2014, 5, 4213] has become an intensively discussed approach that could provide accurate results before the dawn of error-tolerant quantum computing. In this work we present an implementation of UCCSD-VQE that allows for thefirst time to treat both open- and closed-shell molecules. We study the accuracy of the obtained energies for nine small molecular systems as well as for four exemplary chemical reactions by comparing to well-established electronic structure methods like (non-unitary) coupled-cluster and density functional theory. Finally, we roughly estimate the required quantum hardware resources to obtain "useful" results for practical purposes.