Variational quantum imaginary time evolution for matrix product state Ansatz with tests on transcorrelated Hamiltonians.

Abstract

The matrix product state (MPS) Ansatz offers a promising approach for finding the ground state of molecular Hamiltonians and solving quantum chemistry problems. Building on this concept, the proposed technique of quantum circuit MPS (QCMPS) enables the simulation of chemical systems using a relatively small number of qubits. In this study, we enhance the optimization performance of the QCMPS Ansatz by employing the variational quantum imaginary time evolution (VarQITE) approach. Guided by McLachlan's variational principle, the VarQITE method provides analytical metrics and gradients, resulting in improved convergence efficiency and robustness of the QCMPS. We validate these improvements numerically through simulations of H2, H4, and LiH molecules. In addition, given that VarQITE is applicable to non-Hermitian Hamiltonians, we evaluate its effectiveness in preparing the ground state of transcorrelated Hamiltonians. This approach yields energy estimates comparable to the complete basis set (CBS) limit while using even fewer qubits. In particular, we perform simulations of the beryllium atom and LiH molecule using only three qubits, maintaining high fidelity with the CBS ground state energy of these systems. This qubit reduction is achieved through the combined advantages of both the QCMPS Ansatz and transcorrelation. Our findings demonstrate the potential practicality of this quantum chemistry algorithm on near-term quantum devices.