Person:

Kaxiras, Efthimios

We investigate electron and hole dynamics upon photon excitation in dye-sensitized solar cells, using a recently developed method based on real-time evolution of electronic states through time-dependent density functional theory. The systems we considered consist of organic sensitizers and nanocrystalline (TiO_2) semiconductors. We examine the influence of various factors on the dynamics of electrons and holes, including point defects (vacancies) on the (TiO_2) surface, variations in the dye molecular size and binding geometry, and thermal fluctuations which result in different alignments of the electronic energy levels. Two clear trends emerge: (a) dissociated adsorption of the dye molecules leads to faster electron injection dynamics by reducing interfacial dipole moments; (b) oxygen vacancy defects stabilize dye adsorption and facilitate charge injection, at the cost of lower open circuit voltage and higher electron−hole recombination rate. Understanding of these effects at the atomic level suggests tunable parameters through which the electronic characteristics of dye-sensitized solar cell devices can be improved and their efficiency can be maximized.