: In accounting for the magnetic properties of discrete and extended compounds with unpaired spins, it is crucial to know the nature of their ground and low-lying excited states. In this review we surveyed quantum mechanical descriptions on how these states are affected by spin-orbit coupling and attempted to provide a conceptual framework with which to think about spin-orbit coupling and its applications. q 2008 Wiley Periodicals, Inc. J Comput Chem 00: 000