4.8 Article

Quantum Shells Boost the Optical Gain of Lasing Media

Journal

ACS NANO
Volume 16, Issue 2, Pages 3017-3026

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.1c10404

Keywords

nanocrystal; X-ray; light; scintillator; laser diode; biexciton; trion

Funding

  1. U.S. Department of Energy, Office of Science [DE-SC0016872, DE-AC02-06CH11357]
  2. University of Michigan College of Engineering
  3. NSF [DMR-9871177]
  4. U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0021650]
  5. DOE-BES [DE-SC0010697]
  6. U.S. Department of Energy (DOE) [DE-SC0021650, DE-SC0010697] Funding Source: U.S. Department of Energy (DOE)

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The study shows that semiconductor quantum shells with an inverted geometry can inhibit Auger recombination in quantum dots and improve their multiexciton characteristics. By promoting spatial separation between multiple excitons and inducing exciton-exciton repulsion, quantum shells can achieve ultralong lifetimes and high quantum yields, making them attractive for optically and electrically pumped gain media.
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.

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