TD-DFT/B real-time charge dynamics at hybrid interfaces

In a recent work, we have studied the photodynamic process in a supramolecular arrangement composed of a hydrogenated nanodiamond (C190H110) interacting with a 3,4,9,10-perylenetetra-carboxylic acid diimide (PDI) molecule as acceptor. After pulse irradiation in tune with the photoexcitation of the acceptor, the system shows an ultrafast charge transfer process reaching a stable steady state in a few tens of femtoseconds. We proposed a purely electronic reordering of the system after charge separation as the reason for the irreversibility of the process. Also van der Waals heterostructures from layered molecular stacks might offer means to efficient optoelectronics, due to adjustable photoactive, charge separation and collection layers. TD-DFTB simulations reveals nonlinear interlayer exciton dissociation without recombination in perylene acceptors and cove graphene nanoribbon donors on top of armchair graphene platforms.