Single-exciton optical gain in semiconductor nanocrystals

Nanocrystal quantum dots have favourable light-emitting properties. They show photoluminescence with high quantum yields, and their emission colours depend on the nanocrystal size—owing to the quantum-confinement effect—and are therefore tunable. However, nanocrystals are difficult to use in optical amplification and lasing. Because of an almost exact balance between absorption and stimulated emission in nanoparticles excited with single electron–hole pairs (excitons), optical gain can only occur in nanocrystals that contain at least two excitons. A complication associated with this multiexcitonic nature of light amplification is fast optical-gain decay induced by non-radiative Auger recombination, a process in which one exciton recombines by transferring its energy to another. Here we demonstrate a practical approach for obtaining optical gain in the single-exciton regime that eliminates the problem of Auger decay. Specifically, we develop core/shell hetero-nanocrystals engineered in such a way as to spatially separate electrons and holes between the core and the shell (type-II heterostructures). The resulting imbalance between negative and positive charges produces a strong local electric field, which induces a giant (∼100 meV or greater) transient Stark shift of the absorption spectrum with respect to the luminescence line of singly excited nanocrystals. This effect breaks the exact balance between absorption and stimulated emission, and allows us to demonstrate optical amplification due to single excitons. Semiconductor nanocrystals have very good light-emitting properties, so have potential as optical amplification media that can be easily processed with solution-based techniques: possible applications include optical interconnects in microelectronics, lab-on-a-chip technologies and quantum information processing. The problem with these structures is that at least two excitons (bound electron–hole pairs) need to be present in a nanocrystal before optical gain can be achieved, and this limits performance. In effect, the excitons annihilate each other before optical amplification can occur. This obstacle has now been overcome using nanocrystals with cores and shells made from different semiconductor materials, constructed in such a way that electrons and holes are separated from each other. This makes optical gain based on single excitons possible, significantly enhancing their promise as a practical optical material for laser applications. Semiconductor nanocrystals seem good candidates for 'soft' optical gain media, but optical gain and lasing is hard to achieve owing to a fundamental optical effect, which involves the problem that at least two excitons need to be present in a nanocrystal to achieve gain, and this limits performance. Here the problem is circumvented by designing nanocrystals with cores and shells made from different semiconductor materials, and in such a way that electrons and holes are separated from each other: this makes possible optical gain based on single excitons, thereby significantly enhancing the promise of semiconductor nanocrystals as practical optical materials for a wide range of lasing applications.