Propagating multi-dimensional density operators using the multi-layer-ρ multi-configurational time-dependent Hartree method.

Solving the Liouville-von-Neumann equation using a density operator provides a more complete picture of dynamical quantum phenomena than by using a wavepacket and solving the Schrödinger equation. As density operators are not restricted to the description of pure states, they can treat both thermalized and open systems. In practice, however, they are rarely used to study molecular systems as the computational resources required are even more prohibitive than those needed for wavepacket dynamics.