Stimulated Emission and Lasing from Bulk CdSe Nanocrystals

Abstract

Nanocrystals with a size in the regime of vanishing quantum confinement, or bulk nanocrystals (BNCs), have emerged recently as viable solution processable optical gain materials in the green part of the spectrum. Here, we show that these properties can be extended to the crucial red region using CdSe BNCs. Through quantitative time-resolved spectroscopy, we can model these nanocrystals as bulk semiconductors, thereby revealing that the gain originates from an unbound electron−hole plasma state. The gain is broadband in nature and is not capped by Auger processes, but by a slower second-order recombination resulting in nanosecond gain lifetimes. Finally, optically pumped lasers under femtosecond pulsed and quasi-continuous wave operation are demonstrated using a photonic crystal surface emitting laser cavity, thereby stretching from 635 to 720 nm. Our results indicate that compositional variation can indeed provide spectral versatility to the BNC concept, while preserving the excellent gain metrics associated with it.