论文标题
多体分散相互作用的第二个量化方法
Second Quantization Approach to Many-Body Dispersion Interactions
论文作者
论文摘要
多体色散（MBD）框架是一种成功建模具有数千原子系统的远程电子相关能和光学响应的方法。受田间理论的启发，我们在这里开发了第二量化的MBD形式主义（SQ-MBD），该形式（SQ-MBD）在Fock空间表示中重铸了原子量子drude振荡器系统。 SQ-MBD提供了（I）在原子系统的粗粒度表示上投射可观察到的工具（相互作用的能量，过渡性多物，极化张量），范围从单个原子到大型结构基序，（ii）量子信息框架，以分析与给定复合物相关性的相关性和（III II）的相关性，以分析和（不可分割）。有数百万原子。 SQ-MBD方法为分子系统中的量子波动提供了新的见解，并可以直接耦合集体等离子体样的MBD MBD自由度与任意环境，从而提供了可拖动的计算框架，以治疗分散性的相互作用和复杂系统中的极化响应。
The many-body dispersion (MBD) framework is a successful approach for modeling the long-range electronic correlation energy and optical response of systems with thousands of atoms. Inspired by field theory, here we develop a second-quantized MBD formalism (SQ-MBD) that recasts a system of atomic quantum Drude oscillators in a Fock-space representation. SQ-MBD provides (I) tools for projecting observables (interaction energy, transition multipoles, polarizability tensors) on coarse-grained representations of the atomistic system ranging from single atoms to large structural motifs, (ii) a quantum-information framework to analyze correlations and (non)separability among fragments in a given molecular complex, and (iii) a path toward the applicability of the MBD framework to molecular complexes with millions of atoms. The SQ-MBD approach offers novel insights into quantum fluctuations in molecular systems and enables direct coupling of collective plasmon-like MBD degrees of freedom with arbitrary environments, providing a tractable computational framework to treat dispersion interactions and polarization response in intricate systems.
