A microscopic picture of surface charge trapping in semiconductor nanocrystals

Several different compositions of semiconductor nanocrystals are subjected to numerous spectroscopic techniques to elucidate the nature of surface trapping in these systems. We find a consistent temperature-dependent relationship between core and surface photoluminescence intensity and marked differences in electron-phonon coupling for core and surface states based on ultrafast measurements and Resonance Raman studies, respectively. These results support a minimal model of surface charge trapping applicable to a range of nanocrystal systems involving a single surface state in which the trapped charge polarization leads to strong phonon couplings, with transitions between the surface and band edge excitonic states being governed by semiclassical electron-transfer theory.