标题： 真实腔体中的分子极化子动力学 显示英文标题

标题： Molecular polaritons dynamics in realistic cavities

摘要： 在极子化学过程中涉及的自由度数量很大，这由于计算成本高而大大限制了任何从头算方法可以描述的系统。 半经典方法将光作为经典处理，为克服这些限制提供了一条有前景的途径。 在本工作中，我们提出了一种新的实现方法，该方法结合了麦克斯韦方程的数值传播以模拟现实腔体，以及在密度泛函紧束缚（DFTB）理论水平上的量子电子动力学。 这种实现方法允许对大量在原子层面描述的分子进行模拟，这些分子与通过数值求解麦克斯韦方程得到的腔模相互作用。 通过模仿实验设置，我们的方法能够计算透射光谱，在其中我们观察到相应的极子信号。 此外，我们还可以获得局部信息，揭示个体分子的复杂响应，这些响应取决于腔体内分子的数量、几何结构、位置和取向。 显示英文摘要

摘要： The large number of degrees of freedom involved in polaritonic chemistry processes considerably restricts the systems that can be described by any ab initio approach, due to the resulting high computational cost. Semiclassical methods that treat light classically offer a promising route for overcoming these limitations. In this work, we present a new implementation that combines the numerical propagation of Maxwell's equations to simulate realistic cavities with quantum electron dynamics at the density functional tight-binding (DFTB) theory level. This implementation allows for the simulation of a large number of molecules described at the atomistic level, interacting with cavity modes obtained by numerically solving Maxwell's equations. By mimicking experimental setups, our approach enables the calculation of transmission spectra, in which we observe the corresponding polaritonic signals. In addition, we have access to local information, revealing complex responses of individual molecules that depend on the number, geometry, position, and orientation of the molecules inside the cavity.