发表机构
German Aerospace Center (DLR); Helmholtz Institute Ulm; Universität Ulm（德国航空航天中心; 乌尔姆赫尔霍兹研究所; 乌尔姆大学）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
提出一种混合量子-经典算法，通过核-电子轨道方法在量子计算机上纳入核量子效应进行从头算分子动力学，模拟H₂、H₂O和Zundel离子，验证了质子穿梭无势垒及频率误差改善，并展示了在近期量子设备上的可行性。
AI 中文摘要
核量子效应对于描述质子转移和氢键至关重要，但在经典硬件上将其纳入量子化学计算通常在计算上是不可行的。一个有前景的替代方案是量子计算机，因为其对空间的需求随系统尺寸线性扩展。我们提出了一种新颖的混合量子-经典算法，用于从头算分子动力学，通过核-电子轨道方法纳入核量子效应。该算法在量子计算机上使用变分量子本征求解器评估基态能量和力，而分子几何结构则在经典计算机上更新。我们通过对H₂、H₂O和Zundel离子H₅O₂⁺的模拟验证了我们的方法，并将模拟的振动光谱与实验数据进行了比较。在纳入核量子效应后，Zundel离子中的质子穿梭运动变得实际上无势垒，模拟频率的误差也显著改善。采用紧凑的硬件高效拟设电路，我们获得了与更精确的UCCSD拟设相当的结果，这暗示了我们的算法在近期量子设备上执行的可行性。
英文摘要
Nuclear quantum effects are critical for describing proton transfer and hydrogen bonding, but their incorporation into quantum chemistry calculations is often computationally prohibitive on classical hardware. A promising alternative are quantum computers due to their linear scaling in the space requirements with system size. We introduce a novel hybrid quantum-classical algorithm for ab-initio molecular dynamics that incorporates nuclear quantum effects via the nuclear-electronic orbital method. The proposed algorithm evaluates ground state energies and forces on the quantum computer using a variational quantum eigensolver, while the molecular geometries are updated classically. We validate our approach through simulations of $\text{H}_2$, $\text{H}_2\text{O}$ and the Zundel ion $\text{H}_5\text{O}_2^+$, comparing the simulated vibrational spectra with experimental data. Upon inclusion of nuclear quantum effects, the proton shuttling movement in the Zundel ion becomes effectively barrierless, and errors in the simulated frequencies improve significantly. Employing compact hardware-efficient ansatz circuits we achieve results comparable to the more accurate UCCSD ansatzes, which hints towards the feasibility of executing our algorithm on near-term quantum devices.
Comments21 pages, 14 figures
