Sub-single exciton optical gain threshold in colloidal semiconductor quantum wells with gradient alloy shelling

TL;DR

This paper reports the achievement of sub-single exciton optical gain in specially engineered colloidal quantum wells, enabling low-threshold, long-lived optical amplification and a step towards solution-processable colloidal lasers.

Contribution

The study introduces gradient alloy shell engineering in colloidal quantum wells to achieve sub-single exciton optical gain thresholds, reducing Auger recombination effects.

Findings

Achieved sub-single exciton optical gain threshold of Ng=0.80.

Observed amplified spontaneous emission at low pump fluence of 800 nJ/cm².

Demonstrated a colloidal laser with an ultralow lasing threshold of 7.5 μJ/cm².

Abstract

Colloidal semiconductor quantum wells have emerged as a promising material platform for use in solution-processable light-generation including colloidal lasers. However, application relying on their optical gain suffer from a fundamental complication due to multi-excitonic nature of light amplification in common II-VI semiconductor nanocrystals. This undesirably increases the optical gain threshold and shortens the net gain lifetime because of fast nonradiative Auger decay. Here, we demonstrate sub-single exciton level of optical gain threshold in specially engineered CdSe/CdS@CdZnS core/crown@gradient alloyed shell colloidal quantum wells. This sub-single exciton ensemble-averaged gain threshold of Ng = 0.80 (per particle) resulting from impeded Auger recombination along with a large absorption cross-section of quantum wells enables us to observe the amplified spontaneous emission starting at a low pump fluence of 800 nJ cm-2, at least three-folds better than the previously best reported values among all colloidal semiconductor nanocrystals. Moreover, long optical gain lifetimes of 800 ps accompanied with modal gain coefficients of 2,000 cm-1 are achieved. Finally, using these gradient shelled quantum wells, we show a vertical cavity surface-emitting colloidal laser operating at an ultralow lasing threshold of 7.5 micro-joule cm-2. These results represent a significant step towards the realization of solution-processable electrically-driven colloidal lasers.