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

Sander J. W. Vonk, P. Tim Prins, Tong Wang, Jan Matthys, Luca Giordano, Pieter Schiettecatte, Navendu Mondal, Jaco J. Geuchies, Arjan J. Houtepen, Jessi E. S. Hoeven, Thomas R. Hopper, Zeger Hens, Pieter Geiregat, Artem A. Bakulin and Freddy T. Rabouw ()
Additional contact information
Sander J. W. Vonk: Utrecht University
P. Tim Prins: Institute for Sustainable and Circular Chemistry
Tong Wang: Imperial College London
Jan Matthys: Ghent University
Luca Giordano: Ghent University
Pieter Schiettecatte: Ghent University
Navendu Mondal: Imperial College London
Jaco J. Geuchies: Leiden University
Arjan J. Houtepen: Delft University of Technology
Jessi E. S. Hoeven: Debye Institute for Nanomaterials Science
Thomas R. Hopper: Imperial College London
Zeger Hens: Ghent University
Pieter Geiregat: Ghent University
Artem A. Bakulin: Imperial College London
Freddy T. Rabouw: Utrecht University

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: 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 unusual photophysics of state-of-the-art InP-based quantum dots, which makes them unattractive as a laser gain material despite a near-unity quantum yield. 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 reduces the achievable population inversion and limits light amplification for lasing applications. However, it does not quench fluorescence. Instead, trapped carriers can recombine radiatively, leading to delayed—but bright—fluorescence. Single-quantum-dot experiments confirm the direct link between hot-carrier trapping and delayed fluorescence. Hot-carrier trapping thus explains why the latest generation of InP-based quantum dots struggle to support optical gain, although the quantum yield is near unity for low-intensity applications. Comparison with other popular quantum-dot materials—CdSe, Pb–halide perovskites, and CuInS2—indicate that the hot-carrier dynamics observed are unique to InP.

Date: 2025
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DOI: 10.1038/s41467-025-61511-9

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