Delta self-consistent-field methods are widely used in studies of electronically excited states. However, the nonaufbau determinants are generally spin-contaminated. Here, we describe a general approach for spin-coupling interactions of open-shell molecules, making use of multistate density functional theory (MSDFT). In particular, the effective exchange integrals that determine spin coupling are obtained by enforcing the multiplet degeneracy of the S+1 state in the M S = S manifold. Consequently, they are consistent with the energy of the high-spin state that is adequately treated by Kohn−Sham density functional theory (DFT) and, thereby, free of double counting of correlation. The method was applied to core excitations of open-shell molecules and compared with those by spin-adapted timedependent DFT. An excellent agreement with experiment was found employing the BLYP functional and aug-cc-pCVQZ basis set. Overall, MSDFT provides an effective combination of the strengths of DFT and wave function theory to achieve efficiency and accuracy.

The BDF (Beijing Density Functional) program package is in the first place a platform for theoretical and methodological developments, standing out particularly in relativistic quantum chemical methods for chemistry and physics of atoms, molecules, and periodic solids containing heavy elements. These include the whole spectrum of relativistic Hamiltonians and their combinations with density functional theory for the electronic structure of ground states as well as time-dependent and static density functional linear response theories for electronically excited states and electric/magnetic properties. However, not to be confused by its name, BDF nowadays comprises also of standard and novel wave function-based correlation methods for the ground and excited states of strongly correlated systems of electrons [e.g., multireference configuration interaction, static–dynamic–static configuration interaction, static–dynamic–static second-order perturbation theory, n-electron valence second-order perturbation theory, iterative configuration interaction (iCI), iCI with selection plus PT2, and equation-of-motion coupled-cluster]. Additional features of BDF include a maximum occupation method for finding excited states of Hartree–Fock/Kohn–Sham (HF/KS) equations, a very efficient localization of HF/KS and complete active space self-consistent field orbitals, and a unique solver for exterior and interior roots of large matrix eigenvalue problems.

In the presence of a catalytic amount of radical initiator AIBN, primary amines are oxidatively coupled to imines and tertiary amines are cyanated to α-aminonitriles. These "metal-free" aerobic oxidative coupling reactions may find applications in a wide range of "green" oxidation chemistry.

O2 activation in WelO5 (an α-KG dependent halogenase) leads to a Fe(IV)O species with an equatorial conformation. After hydrogen abstraction, the hydroxyl ligand is far from the substrate radical which leads to the chlorination selectivity