AI 中文总结
该研究提出了结合LUCJ拟设与SQD的量子-经典工作流，可在气相及显式溶剂QM/MM模拟中准确重现FCI的能量、梯度等结果，为量子硬件集成到QM/MM分子动力学提供了实用途径。
AI 中文摘要
我们展示了一种用于从头算分子动力学（AIMD）的量子-经典工作流，其中源自化学启发的LUCJ拟设的量子测量结果，采用基于样本的量子对角化（SQD）进行后处理，以恢复行列式子空间并提供动力学所需的能量和解析核梯度。作为精确基准，我们在STO-3G基组下使用全组态相互作用（FCI），实现了对SQD准确性的直接评估。在气相基准测试中，SQD重现的FCI能量和梯度与FCI参考值的偏差在1 kcal mol⁻¹以内，并产生稳定的AIMD轨迹。在显式溶剂化的QM/MM模拟中，SQD仍保持这种一致性，与FCI能量波动、RMS梯度剖面匹配，并通过径向分布函数量化重现溶质-溶剂结构。总体而言，这些基准测试确立了LUCJ+SQD是将当前量子硬件集成到QM/MM分子动力学中的实用途径，并提供了由量子电子结构引擎驱动的凝聚相QM/MM动力学的早期演示。
英文摘要
We demonstrate a quantum-classical workflow for ab initio molecular dynamics (AIMD) in which quantum measurements from a chemistry-inspired LUCJ ansatz are post-processed using Sample-based Quantum Diagonalization (SQD) to recover determinant subspaces and deliver energies and analytical nuclear gradients for dynamics. As an exact benchmark, we use full configuration interaction (FCI) in the STO-3G basis, enabling a direct assessment of the accuracy of SQD. In gas-phase benchmarks, SQD reproduces FCI energies and gradients to within 1 kcal mol$^{-1}$ of the FCI reference and yields stable AIMD trajectories. In explicit-solvent QM/MM simulations, SQD retains this agreement, matching FCI energy fluctuations and RMS gradient profiles and reproducing solute-solvent structure as quantified by radial distribution functions. Overall, these benchmarks establish LUCJ+SQD as a practical route for integrating current quantum hardware into QM/MM molecular dynamics and provide an early demonstration of condensed-phase QM/MM dynamics driven by a quantum electronic-structure engine.
Comments45 pages, 7 figures. Supporting Information included as an ancillary file
