Hot-Carrier Trapping Preserves High Quantum Yields but Limits Optical Gain in InP-Based Quantum Dots
Freddy Rabouw a, Sander Vonk a, Tim Prins a, Tong Wang b, Jan Matthys c, Luca Giordano c, Pieter Schiettecatte c, Navendu Mondal b, Jessi van der Hoeven a, Thomas Hopper b, Zeger Hens c, Pieter Geiregat c, Artem Bakulin b
a Debye Institute for Nanomaterials Science, Utrecht University, Heidelberglaan, 8, Utrecht, Netherlands
b Department of Chemistry and Centre for Processable Electronics, Imperial College London, London W12 0BZ, United Kingdom.
c Physics and Chemistry of Nanostructures Group, Ghent University, 9000 Ghent, Belgium
Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)
#PhotoQD - Photophysics of colloidal quantum dots
Lausanne, Switzerland, 2024 November 12th - 15th
Organizers: Philippe Green and Jannika Lauth
Invited Speaker, Freddy Rabouw, presentation 276
Publication date: 28th August 2024

The development of high-quality QDs with tunable visible emission started with CdSe. QD designs containing Cd or Pb remain those with the brightest emission and most precise control over properties. However, as consumer applications demand QDs free of toxic elements, alternative materials have drawn considerable attention in recent years. InP-based QDs now offer photoluminescence efficiencies and a color tunability that are on par with those of high-quality Cd- and Pb-containing designs. This makes InP-based QDs an ideal phosphor for displays and lighting.

In stark contrast to these successes, InP-based QDs struggle in more demanding optical applications. In particular, the development of QD lasers using InP-based QDs lags behind other QD materials by more than two decades. Lasing from InP-based QDs has been reported only once, while the vast majority of the QD lasing literature has successfully used Cd-based or Pb-halide perovskite QDs. The near-total absence of InP-based QDs in the lasing literature is consistent with spectroscopic measurements, which have highlighted difficulties to achieve population inversion and gain from an ensemble of InP-based QDs.

In this presentation, I will show ensemble and single-particle experiments to investigate why InP-based QDs are not yet suitable for lasing applications, despite their high brightness, and how their performance may be improved. On the ensemble level, we find a correlation between the magnitude of charge-carrier losses on the sub-ps timescales and slow delayed emission on the ns-to-μs timescales. From single-particle measurements, we find a cause–effect relationship between hot-carrier trapping and delayed trap emission. Based on the characteristics of the trap-related emission, we propose that hot-carrier traps are most likely internal defects, for example located on the InP/ZnSe interface. This highlights the direction into which InP-based QDs should be improved for next-generation applications.

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