比较半经典平均场与1-激子近似在强光-物质耦合条件下评估光学响应
Comparing semiclassical mean-field and 1-exciton approximations in evaluating optical response under strong light-matter coupling conditions
AI总结：
本文比较了强光-物质耦合下1-激子近似与半经典平均场近似评估光学响应的结果，发现两者在原型问题上高度一致。
摘要：
许多分子与辐射场集体相互作用的严格量子力学描述通常被认为在数值上难以处理，必须采用近似方案。标准光谱学通常包含一定级别的微扰理论，但在强耦合条件下，会使用其他近似。一种常见的近似是1-激子模型，其中涉及弱激发的过程使用由分子腔模系统的基态和单激发态组成的基矢来描述。在数值研究中另一种常用的近似中，电磁场被经典地描述，量子分子子系统在平均场Hartree近似中处理，其波函数假设为单分子波函数的乘积。前者忽略了需要长时间才能布居的状态，因此本质上是一种短时间近似。后者不受此限制，但就其本质而言，忽略了某些分子间和分子-场关联。在本工作中，我们直接比较了将这些近似应用于涉及分子-光学腔系统中光学响应的几个原型问题时所获得的结果。特别是，我们展示了我们最近使用截断的1-激子近似对电子强耦合与分子核动力学之间相互作用进行的模型研究（J. Chem. Phys. 157, 114108 (2022)）与半经典平均场计算非常吻合。
英文摘要：
The rigorous quantum mechanical description of the collective interaction of many molecules with the radiation field is usually considered numerically intractable, and approximation schemes must be employed. Standard spectroscopy usually contains some levels of perturbation theory, but under strong coupling conditions, other approximations are used. A common approximation is the 1-exciton model in which processes involving weak excitations are described using a basis comprising of the ground state and singly excited states of the molecule cavity-mode system. In another frequently used approximation in numerical investigations, the electromagnetic field is described classically, and the quantum molecular subsystem is treated in the mean-field Hartree approximation with its wavefunction assumed to be a product of single molecules' wavefunctions. The former disregards states that take long time to populate, and is therefore essentially a short time approximation. The latter is not limited in this way, but by its nature, disregards some intermolecular and molecule-field correlations. In this work, we directly compare results obtained from these approximations when applied to several prototype problems involving the optical response of molecule-in-optical cavities systems. In particular, we show that our recent model investigation (J. Chem. Phys. 157, 114108 (2022)) of the interplay between the electronic strong coupling and molecular nuclear dynamics using the truncated 1-exciton approximation agrees very well with the semiclassical mean-field calculation.
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