Study of the photodissociation of a CdSe nanocrystal beam by means of photoluminescence and Raman scattering

Abstract

We developed an apparatus that enables us to perform optical measurements of nanocrystals suspended in vacuum. CdSe nanocrystals were produced by a gas evaporation method, and nanocrystal beams were then formed using an inert-gas flow with differential pumping. We measured photoluminescence spectra of the nanocrystal beams with excitations of various photon energies and powers. For a low excitation power, edge emission of the CdSe nanocrystal beam was observed. With increase of the laser power, Raman lines of Se dimers emitted due to the photodissociation of CdSe nanocrystals were observed. It was found that the thresholds of the excitation laser fluence for the photodissociation of CdSe nanocrystals were much smaller than the thresholds of laser fluence for the laser-induced emission of Se atoms from bulk CdSe. The electronic process is dominant in the photodissociation of CdSe nanocrystals whose surfaces are completely free. We suggest that the effective supply of carriers confined in nanocrystals to the surface state, and the excitations of the completely free surface state induce the photodissociation of nanocrystals by excitation with much weaker irradiation than is required for dissociation of the bulk surface.