Coupled Cluster Method with Single and Double Excitations Tailored by Matrix Product State Wave Functions.
In the past decade, the quantum chemical version of the density matrix renormalization group (DMRG) method has established itself as the method of choice for calculations of strongly correlated molecular systems. Despite its favorable scaling, it is in practice not suitable for computations of dynamic correlation. We present a novel method for accurate "post-DMRG" treatment of dynamic correlation based on the tailored coupled cluster (CC) theory in which the DMRG method is responsible for the proper description of nondynamic correlation, whereas dynamic correlation is incorporated through the framework of the CC theory. We illustrate the potential of this method on prominent multireference systems, in particular, N2and Cr2molecules and also oxo-Mn(Salen), for which we have performed the first post-DMRG computations in order to shed light on the energy ordering of the lowest spin states.
J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic , v.v.i., Dolejškova 3, 18223 Prague 8, Czech Republic.
Libor
L
Veis
J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic , v.v.i., Dolejškova 3, 18223 Prague 8, Czech Republic.
Andrej
A
Antalík
J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic , v.v.i., Dolejškova 3, 18223 Prague 8, Czech Republic.
Jiří
J
Brabec
Max Planck Institut für Chemische Energiekonversion , Stiftstrasse 34-36, D-45470 Mülheim an der Ruhr, Germany.
Frank
F
Neese
Strongly Correlated Systems "Lendület" Research Group, Wigner Research Centre for Physics , H-1525 Budapest, Hungary.
Örs
Ö
Legeza
J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic , v.v.i., Dolejškova 3, 18223 Prague 8, Czech Republic.
Jiří
J
Pittner