Department of Chemistry and Biochemistry, University of California at Los Angeles, Los Angeles, California 90095-1569, USA.
J Chem Phys. 2012 Aug 21;137(7):074113. doi: 10.1063/1.4745847.
We develop an approach for dynamical (ω > 0) embedding of mixed quantum mechanical (QM)/classical (or more precisely QM/electrodynamics) systems with a quantum sub-region, described by time-dependent density functional theory (TDDFT), within a classical sub-region, modeled here by the recently proposed near-field (NF) method. Both sub-systems are propagated simultaneously and are coupled through a common Coulomb potential. As a first step we implement the method to study the plasmonic response of a metal film which is half jellium-like QM and half classical. The resulting response is in good agreement with both full-scale TDDFT and the purely classical NF method. The embedding method is able to describe the optical response of the whole system while capturing quantum mechanical effects, so it is a promising approach for studying electrodynamics in hybrid molecules-metals nanostructures.
我们开发了一种方法，用于在经典子区域（这里通过最近提出的近场（NF）方法建模）中对具有量子子区域的混合量子力学（QM）/经典（或更确切地说 QM/电动力学）系统进行动力学（ω>0）嵌入，该量子子区域由时变密度泛函理论（TDDFT）描述。两个子系统同时传播，并通过公共库仑势耦合。作为第一步，我们实施该方法来研究金属膜的等离子体响应，该金属膜一半是类凝胶 QM，一半是经典的。得到的响应与全规模 TDDFT 和纯粹的经典 NF 方法都非常吻合。嵌入方法能够描述整个系统的光学响应，同时捕获量子力学效应，因此它是研究混合分子-金属纳米结构中电动力学的一种很有前途的方法。
