在超导量子处理器上模拟锍离子基态与激发态性质的量子化学
Quantum chemistry simulation of ground- and excited-state properties of the sulfonium cation on a superconducting quantum processor
AI总结：
本研究在 IBM Falcon 超导量子处理器上模拟 H$_3$S$^+$ 分子电子结构，通过推广纠缠锻造（EF）量子比特缩减技术与量子子空间展开结合，并部署误差缓解，成功计算基态与激发态势能曲线的偶极结构因子等性质，揭示了光致碎裂路径，为近期量子设备模拟光解反应迈出重要一步。
摘要：
对关联电子结构，特别是多电子系统激发态的计算描述，是量子设备的一个预期应用。一个重要的应用分支是确定光敏化合物（如光刻胶中使用的基于锍的光酸产生剂）在光解实验中占主导的分子碎裂路径。在此，我们在 IBM Falcon 架构的超导量子处理器上模拟了 H$_3$S$^+$ 分子的静态和动态电子结构，将其作为三键合硫阳离子的最小模型。为此，我们将一种量子比特缩减技术（称为纠缠锻造或 EF [A. Eddins 等人，Phys. Rev. X Quantum, 3, 010309 (2022)]）进行推广，该技术目前仅限于评估基态能量，现已扩展至分子性质的处理。在传统量子模拟中，一个量子比特代表一个自旋轨道，而在 EF 中，一个量子比特代表一个空间轨道，从而将所需量子比特数减少一半。我们将广义 EF 与量子子空间展开 [W. Colless 等人，Phys. Rev. X 8, 011021 (2018)] 相结合，这是一种用于在子空间中投影基态和激发态的不含时薛定谔方程的技术。为了实现该算法工作流的实验演示，我们部署了一系列误差缓解技术。我们计算了沿基态和激发态势能曲线的偶极结构因子和部分原子电荷，揭示了同源和异源碎裂的发生。这项研究是迈向在近期量子设备上计算描述光解过程的重要一步，因为它可以推广到其他光解过程，并能以不同方式自然扩展以实现更真实的模拟。
英文摘要：
The computational description of correlated electronic structure, and particularly of excited states of many-electron systems, is an anticipated application for quantum devices. An important ramification is to determine the dominant molecular fragmentation pathways in photo-dissociation experiments of light-sensitive compounds, like sulfonium-based photo-acid generators used in photolithography. Here we simulate the static and dynamic electronic structure of the H$_3$S$^+$ molecule, taken as a minimal model of a triply-bonded sulfur cation, on a superconducting quantum processor of the IBM Falcon architecture. To this end, we generalize a qubit reduction technique termed entanglement forging or EF [A. Eddins et al., Phys. Rev. X Quantum, 3, 010309 (2022)], currently restricted to the evaluation of ground-state energies, to the treatment of molecular properties. While, in a conventional quantum simulation, a qubit represents a spin-orbital, within EF a qubit represents a spatial orbital, reducing the number of required qubits by half. We combine the generalized EF with quantum subspace expansion [W. Colless et al, Phys. Rev. X 8, 011021 (2018)], a technique used to project the time-independent Schrodinger equation for ground and excited states in a subspace. To enable experimental demonstration of this algorithmic workflow, we deploy a sequence of error-mitigation techniques. We compute dipole structure factors and partial atomic charges along the ground- and excited-state potential energy curves, revealing the occurrence of homo- and heterolytic fragmentation. This study is an important step toward the computational description of photo-dissociation on near-term quantum devices, as it can be generalized to other photodissociation processes and naturally extended in different ways to achieve more realistic simulations.
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