Figure 2.

Energies and populations of a dynamics simulation with a model system showing the necessity of doing phase corrections to the matrix U. The left panel shows the energies of the six involved states, ordered by energy as is done in Surface Hopping including ARbitrary Couplings (SHARC). Note that in the panel, the energy differences between the multiplet components are arbitrarily increased for clarity; in the computations, they were degenerate. The middle panel shows the evolution of the populations when phase tracking is performed with the old tracking algorithm in SHARC. The right panel shows the populations with the new tracking algorithm of SHARC2.0, delivering the expected result that at the crossing points complete population transfer occurs between the crossing state pairs, whereas the other states are not affected