Lateral interactions between carbon monoxide molecules adsorbed on a copper Cu(100) surface are investigated via semiclassical initial value representation (SC-IVR) molecular dynamics. A previous analytical potential is extended to include long-range dipole interactions between coadsorbed molecules and preliminary classical simulations were performed to tune the potential parameters. Then, the spectra for several coadsorbed molecules are calculated using the multiple coherent states approximation of the time-averaging representation of the SC-IVR propagator. Results show strong resonances between coadsorbed molecules as observed by past experiments. Resonances turn into dephasing when isotopical substitutions are performed.

The X(2)Σ ground and the A(2)Π and B(2)Σ first two excited states of Li-He and Na-He are determined using high level complete active space self-consistent field-multireference configuration interaction ab initio method. The obtained potentials differ from the ones proposed by Pascale [Phys. Rev. A 28, 632 (1983)], more strongly for the ground than for the excited states. Quantum diffusion Monte Carlo studies of small Li(∗)He(n) and Na(∗)He(n) with n ≤ 5 are performed using a diatomics-in-molecule approach to model the non-pair additive interaction potential. The sensitivity of our results to the A(2)Π and B(2)Σ potentials used is assessed by an analysis of the structure and of the energetics of the clusters. For these small clusters, the physical conclusions are essentially independent of the diatomic curves employed.

Quantum dynamical simulations are essential for a molecular-level understanding of light-induced processes in optoelectronic materials, but they tend to be computationally demanding. We introduce an efficient mixed quantum-classical nonadiabatic molecular dynamics method termed eXcitonic state-based Surface Hopping (X-SH), which propagates the electronic Schrödinger equation in the space of local excitonic and charge-transfer electronic states, coupled to the thermal motion of the nuclear degrees of freedom. The method is applied to exciton decay in a 1D model of a fullerene–oligothiophene junction, and the results are compared to the ones from a fully quantum dynamical treatment at the level of the Multilayer Multiconfigurational Time-Dependent Hartree (ML-MCTDH) approach. Both methods predict that charge-separated states are formed on the 10–100 fs time scale via multiple “hot-exciton dissociation” pathways. The results demonstrate that X-SH is a promising tool advancing the simulation of photoexcited processes from the molecular to the true nanomaterials scale.