Carrier multiplication between interacting nanocrystals for fostering silicon-based photovoltaics

The conversion of solar radiation into electric current with high efficiency is one of the most important topics of modern scientific research, as it holds great potential as a source of clean and renewable energy. Exploitation of interaction between nanocrystals seems to be a promising route to the establishment of third-generation photovoltaics. Here, we adopt a fully ab initio scheme to estimate the role of nanoparticle interplay in the carrier multiplication dynamics of interacting silicon nanocrystals. Energy and charge transfer-based carrier multiplication events are studied as a function of nanocrystal separation, demonstrating the benefits induced by the wavefunction sharing regime. We prove the relevance of these recombinative mechanisms for photovoltaic applications in the case of silicon nanocrystals arranged in dense arrays, quantifying at an atomic scale which conditions maximize the outcome