AI 中文总结
研究利用EWF-(FCI,SQD)方法进行几何优化，将模拟扩展到较大分子，无需碎片化处理，底层片段SQD模拟用70个量子比特，所得几何结构精度高，偏差低于4皮米，为复杂化学过程研究提供新工具。
AI 中文摘要
EWF-(FCI,SQD)方法是一种基于波函数的嵌入方法，结合了全组态相互作用(FCI)和基于样本的量子对角化(SQD)，是模拟分子系统的一种有前途的新工具。然而，EWF-(FCI,SQD)的应用目前仅限于单点计算，而复杂化学过程的研究需要探索势能面的能力。在这项工作中，我们展示了使用EWF-(FCI,SQD)进行几何优化，将模拟扩展到STO-3G基组内的薄荷酮和联苯胺等大分子。在不进行碎片化的情况下，这些系统分别包含73和82个分子轨道，为传统的精确或高级子空间求解器提供了一个难以处理的希尔伯特空间，并明确了基于碎片化方法的必要性。EWF-(FCI,SQD)几何优化中的底层片段SQD模拟使用了多达70个量子比特。相对于经典参考，所得几何结构显示出极高的精度，偏差低于4皮米。
英文摘要
The EWF-(FCI,SQD) method, a wave-function-based embedding approach combining full configuration interaction (FCI) and sample-based quantum diagonalization (SQD), is a promising new tool for the simulation of molecular systems. However, applications of EWF-(FCI,SQD) have so far been limited to single-point calculations, whereas the study of complex chemical processes requires the ability to explore potential energy surfaces. In this work, we demonstrate geometry optimization with EWF-(FCI,SQD), scaling our simulations to molecules as large as menthone and benzidine within the STO-3G basis set. Without fragmentation, these systems comprise 73 and 82 molecular orbitals respectively, presenting an intractable Hilbert space for conventional exact or high-level subspace solvers and establishing a clear necessity for fragmentation-based methodologies. The underlying fragment SQD simulations in the EWF-(FCI,SQD) geometry optimizations use up to 70 qubits. The resulting geometries show exceptional accuracy relative to the classical reference, with deviations below 4 picometers.
