Quantum Shells Boost the Optical Gain of Lasing Media

ACS Nano. 2022 Feb 22;16(2):3017-3026. doi: 10.1021/acsnano.1c10404. Epub 2022 Feb 7.

Abstract

Auger decay of multiple excitons represents a significant obstacle to photonic applications of semiconductor quantum dots (QDs). This nonradiative process is particularly detrimental to the performance of QD-based electroluminescent and lasing devices. Here, we demonstrate that semiconductor quantum shells with an "inverted" QD geometry inhibit Auger recombination, allowing substantial improvements to their multiexciton characteristics. By promoting a spatial separation between multiple excitons, the quantum shell geometry leads to ultralong biexciton lifetimes (>10 ns) and a large biexciton quantum yield. Furthermore, the architecture of quantum shells induces an exciton-exciton repulsion, which splits exciton and biexciton optical transitions, giving rise to an Auger-inactive single-exciton gain mode. In this regime, quantum shells exhibit the longest optical gain lifetime reported for colloidal QDs to date (>6 ns), which makes this geometry an attractive candidate for the development of optically and electrically pumped gain media.

Keywords: X-ray; biexciton; laser diode; light; nanocrystal; scintillator; trion.