Relaxed active space: fixing tailored-CC with high order coupled cluster. II.

Due to the steep increase in computational cost with the inclusion of higher-connected cluster operators in coupled-cluster applications, it is usually not practical to use such methods for larger systems or basis sets without an active space partitioning. This study generates an active space subject to unambiguous statistical criteria to define a space whose size permits treatment at the CCSDT level. The automated scheme makes it unnecessary for the user to judge whether a chosen active space is sufficient to correctly solve the problem. Two demanding applications are presented: twisted ethylene and the transition states for the bicyclo[1,1,0]butane isomerization. As bi-radicals both systems require at least a CCSDT level of theory for quantitative results, for the geometries and energies.