Second harmonic generation and two-photon luminescence upconversion in glasses doped with ZnSe nanocrystalline quantum dots

We report two-photon excited emission in borosilicate glasses doped with ZnSe nanocrystalline quantum dots. The emission, predominantly near the two-photon energy and detected in the direction of the excitation beam, is in the visible, and the fundamental excitation is the near-infrared output of a tunable femtosecond laser. Depending on the two-photon energy, time- and frequency-resolved measurements at room temperature reveal that the emission largely consists of second harmonic generation (SHG) and two-photon luminescence upconversion, and a much smaller luminescence from redshifted, low-lying trap states and other trap levels residing near the semiconductor band edge. We discuss the SHG origin in terms of bulk-like and surface contributions from the nanocrystals and the two-photon resonant enhancement near the excitonic absorption.