The question of how to describe the crossing of molecular electronic states is one of the most challenging issues in contemporary chemical dynamics. In recent years, the fundamental concept of conical intersections (CIs) of electronic potential energy surfaces (PESs) has emerged, which allows extremely fast and efficient switching of a molecule between its excited and ground electronic states. CIs are ubiquitous in polyatomic molecules. Because they generically allow the crossings of the Born−Oppenheimer (BO) adiabatic PESs, they have become the crucial mechanistic elements of the rapidly growing area of nonadiabatic chemistry. The most critical consequence of CIs is a complete breakdown of the adiabatic BO approximation. That means that the reorganization of fast-moving electrons and nuclear vibrations must be treated concurrently. Ideally, the theoretical description should be quantum mechanical in this situation. However, because of the complexity, the necessary approximations often make it difficult to conclusively predict dynamic behavior of large polyatomic molecules. In addition, a nonunique diabatic electronic representation (describing coupling between states in the electronic Hamiltonian) is essential to avoid the singular nature of the nuclear kinetic coupling terms of the unique adiabatic electronic representation.