Scuola Normale Superiore, Piazza dei Cavalieri 7, 56126 Pisa, Italy.
Department of Chemistry, Norwegian University of Science and Technology, 7491 Trondheim, Norway.
J Chem Theory Comput. 2021 Feb 9;17(2):791-803. doi: 10.1021/acs.jctc.0c00940. Epub 2021 Jan 15.
Following recent developments in multilevel embedding methods, we introduce a novel density matrix-based multilevel approach within the framework of density functional theory (DFT). In this multilevel DFT, the system is partitioned in an active and an inactive fragment, and all interactions are retained between the two parts. The decomposition of the total system is performed upon the density matrix. The orthogonality between the two parts is maintained by solving the Kohn-Sham equations in the MO basis for the active part only, while keeping the inactive density matrix frozen. This results in the reduction of computational cost. We outline the theory and implementation and discuss the differences and similarities with state-of-the-art DFT embedding methods. We present applications to aqueous solutions of methyloxirane and glycidol.
基于近年来多尺度嵌入方法的发展，我们在密度泛函理论（DFT）的框架内引入了一种新的基于密度矩阵的多尺度方法。在这种多尺度 DFT 中，系统被分为活性和非活性片段，并且两部分之间保留所有相互作用。总系统的分解是在密度矩阵上进行的。通过仅在活性部分的 MO 基中求解 Kohn-Sham 方程来保持两部分之间的正交性，同时保持非活性密度矩阵冻结。这导致计算成本降低。我们概述了理论和实现，并讨论了与最先进的 DFT 嵌入方法的差异和相似之处。我们介绍了应用于甲基氧化丙烯和缩水甘油的水溶液的情况。
