AI 中文总结
该研究针对多态反应中心化学，构建与反应坐标相关的有效哈密顿量，经映射用耦合修剪和一阶Trotter化在囚禁离子硬件演示工作流程，建立评估框架，展示多态电子动力学，可验证简化哈密顿量。
AI 中文摘要
我们引入布居转移动力学，作为多态反应中心化学中活性空间衍生的简化哈密顿量的实际验证可观测量。使用细胞色素P450启发的铁络合物模型，我们从状态平均完全活性空间自洽场（SA-CASSCF）计算构建与反应坐标相关的有效哈密顿量，将其映射到适合当前硬件的量子电路表示，并从反应物侧基态传播动力学。简化哈密顿量以0.030 eV的均方根偏差和0.143 eV的最大绝对偏差再现SA-CASSCF参考。作为基于动力学的诊断，产物流形布居p_P(t)识别出x = 0.3附近明显的近简并区域，此处状态混合最强。经典精确时间演化在10 fs后于x = 0.3处产生0.488的产物布居，而在x = 0.2处为7.26×10^-2，在x = 0.0处为5.90×10^-3。为了能在当前囚禁离子硬件上执行，我们通过耦合修剪和一阶 Trotter 化研究动力学保真度和电路资源之间的权衡。0.02 eV的耦合截止将非零耦合集从32减少到7，同时保留主要转移路径，M = 30提供了最佳实际操作点。最后，我们在Quantinuum的囚禁离子量子计算机Reimei上演示了该工作流程。硬件再现了经典模型确定的关键反应坐标趋势，包括x = 0.3处的最大值，此处硬件上测量的产物布居为0.42，匹配模拟器上为0.43。这项工作建立了一个基于动力学的框架来评估活性空间衍生的简化哈密顿量，并在当前囚禁离子硬件上展示了具有化学可解释性的多态电子动力学。
英文摘要
We introduce population-transfer dynamics as a practical validation observable for active-space-derived reduced Hamiltonians in multistate reaction-center chemistry. Using a cytochrome P450-inspired Fe-complex model, we construct a reaction-coordinate-dependent effective Hamiltonian from state-averaged complete active-space self-consistent field (SA-CASSCF) calculations, map it to a quantum-circuit representation suitable for current hardware, and propagate dynamics from the reactant-side ground state. The reduced Hamiltonian reproduces the SA-CASSCF reference with an RMS deviation of 0.030 eV and a maximum absolute deviation of 0.143 eV. As a dynamics-based diagnostic, the product-manifold population p_P(t) identifies a pronounced near-degeneracy region around x = 0.3, where state mixing is strongest. Classical exact time evolution yields a product population of 0.488 at x = 0.3 after 10 fs, compared with 7.26 x 10^-2 at x = 0.2 and 5.90 x 10^-3 at x = 0.0. To enable execution on current trapped-ion hardware, we examine the trade-off between dynamical fidelity and circuit resources through coupling pruning and first-order Trotterization. A coupling cutoff of 0.02 eV reduces the non-zero coupling set from 32 to 7 while preserving the dominant transfer pathways, and M = 30 provides the best practical operating point. Finally, we demonstrate the workflow on Quantinuum's trapped-ion quantum computer Reimei. The hardware reproduces the key reaction-coordinate trend identified by the classical model, including the maximum at x = 0.3, where the measured product population is 0.42 on hardware and 0.43 on the matched emulator. This work establishes a dynamics-based framework for assessing active-space-derived reduced Hamiltonians and demonstrates chemically interpretable multistate electronic dynamics on current trapped-ion hardware.
Comments15 pages, 12 figures; Updated acknowledgments and funding information to match the submitted manuscript. No changes to the scientific results or conclusions
