Full quantum mechanical molecular dynamics using Gaussian wavepackets

We present the first application of a promising new method for quantum dynamics calculations. Based on the efficient multiconfiguration time-dependent Hartree wavepacket propagation algorithm, it can treat part, or all, of the wavepacket using Gaussian functions. The Gaussian parameters evolve using variational, coupled equations of motion. In this way the Gaussian basis functions evolve so as to optimally describe the wavepacket. Here, a four-dimensional Henon–Heiles potential surface is used to demonstrate that only a few Gaussian functions are required, and convergence on the full quantum mechanical result is rapid.