The density matrix renormalization group (DMRG) method has already proved itself as a very efficient and accurate computational method, which can treat large active spaces and capture the major part of strong correlation. Its application on larger molecules is, however, limited by its own computational scaling as well as demands of methods for treatment of the missing dynamical electron correlation. In this work, we present the first step in the direction of combining DMRG with density functional theory (DFT), one of the most employed quantum chemical methods with favorable scaling, by means of the projection-based wave function (WF)-in-DFT embedding. On two proof-of-concept but important molecular examples, we demonstrate that the developed DMRG-in-DFT approach provides a very accurate description of molecules with a strongly correlated fragment.

Center for Computational Quantum Physics Flatiron Institute 162 5th Avenue New York 10010New York United States

Faculty of Mathematics and Physics Charles University 121 16Prague Czech Republic

Institute of Physics Lodz University of Technology ul Wolczanska 217 221 93 005Lodz Poland

J Heyrovský Institute of Physical Chemistry Academy of Sciences of the Czech Republic v v i Dolejškova 3 18223Prague 8 Czech Republic

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