Advancing Practical Quantum Embedding Simulations via Operator Commutativity Based State Preparation for Complex Chemical Systems

Abstract

Determining the exponentially scaled ground state wavefunction and the associated molecular properties remains one of the central challenges in quantum chemistry. Hybrid quantum-classical algorithms implemented on quantum computers offer a promising route toward addressing this problem. However, despite several successful demonstrations on small molecular systems, accurate simulations of large and chemically realistic molecules remain difficult due to the limited capability of noisy intermediate scale quantum (NISQ) hardware. To bypass the limitations of NISQ devices, while simultaneously retaining the accuracy of the ground state energy estimations, we propose a dynamic ansatz construction strategy based on operator commutativity and energy driven screening within density matrix embedding theory (DMET) framework. The partitioning of the full system allows us to dynamically construct the ansatz over individual embedded subsystems, allowing each embedding problem be solved individually to a desired accuracy. The embedding Hamiltonian is updated in a self-consistent manner with dynamically formulated wavefunction, and their coupled optimization leads to accurate and efficient description of the overall system. To assess the performance of this approach, we apply it to several molecular systems and chemical processes with up to 144 qubits. These simulations require at most 20 qubits at a time and demonstrate improved accuracy and significantly reduced quantum gate requirements compared with conventional ansatze. We further investigate the impact of various fragmentation strategies and demonstrate the adaptability of our approach at each step of the DMET self-consistency cycle that leads to significantly improved accuracy for strongly correlated system.