  One of the key challenges of quantum-chemical multi-configuration methods is
the necessity to manually select orbitals for the active space. This selection
requires both expertise and experience and can therefore impose severe
limitations on the applicability of this most general class of ab initio
methods. A poor choice of the active orbital space may yield even qualitatively
wrong results. This is obviously a severe problem, especially for wave function
methods that are designed to be systematically improvable. Here, we show how
the iterative nature of the density matrix renormalization group combined with
its capability to include up to about one hundred orbitals in the active space
can be exploited for a systematic assessment and selection of active orbitals.
These benefits allow us to implement an automated approach for active orbital
space selection, which can turn multi-configuration models into black box
approaches.
