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Hot-carrier trapping preserves high quantum yields but limits optical gain in InP-based quantum dots

Materials Science 2024-12-02 v1 Mesoscale and Nanoscale Physics

Abstract

Indium phosphide is the leading material for commercial applications of colloidal quantum dots. To date, however, the community has failed to achieve successful operation under strong excitation conditions, contrasting sharply with other materials. Here, we report how the unusual photophysics of state-of-the-art InP-based quantum dots make them unattractive as a gain material. A combination of ensemble-based time-resolved spectroscopy over timescales from femtoseconds to microseconds and single-quantum-dot spectroscopy reveals ultrafast trapping of hot charge carriers. This process leads to charge-carrier losses, thereby reducing the achievable population inversion which limits amplification of light in a gain material. Interestingly, fluorescence is only delayed, not quenched, by hot charge-carrier trapping, explaining why InP-based quantum dots are successful as bright luminescent colour convertors for low-intensity applications. Comparison with other popular quantum-dot materials, such as CdSe, Pb-halide perovskites, and CuInS2, indicate that the hot-carrier dynamics observed are unique to InP.

Keywords

Cite

@article{arxiv.2411.19565,
  title  = {Hot-carrier trapping preserves high quantum yields but limits optical gain in InP-based quantum dots},
  author = {Sander J. W. Vonk and P. Tim Prins and Tong Wang and Jan Matthys and Luca Giordano and Pieter Schiettecatte and Navendu Mondal and Jessi E. S. van der Hoeven and Thomas R. Hopper and Zeger Hens and Pieter Geiregat and Artem A. Bakulin and Freddy T. Rabouw},
  journal= {arXiv preprint arXiv:2411.19565},
  year   = {2024}
}