Publication date: 21st July 2025
Recently, nanocrystals (NCs) in the regime of vanishing quantum confinement—referred to as bulk nanocrystals (BNCs)—have demonstrated remarkable optical gain characteristics.[1,2] While bulk semiconductor models have successfully explained their high-power lasing behavior, the validity of these models in the low-density regime—where the number of charge carriers per nanocrystal volume becomes discrete—remains an open question. In this study, we investigate the dynamics and energetics of well-defined excited states containing 1 or 2 holes and up to 4 electrons using single-photon avalanche diode (SPAD) array technology. We observe emission from two discrete energy levels for each of the six isolated excited states, indicative of thermal excitation. To validate this thermal behavior, we investigate the temperature-dependent emission characteristics of dozens of individual quantum dots, simultaneously, using multi-particle spectroscopy. This analysis reveals a quantitative match with Boltzmann statistics. By combining the particle-in-a-box approach with Boltzmann population distributions, we develop a model that captures the dynamics and energetics of nanocrystals across the full range from strong quantum confinement to the bulk limit. This work thereby provides a framework for understanding the optical behavior of NCs in the transitional regime between quantum confined and bulk-like, which becomes increasingly relevant as these materials are gaining more prominence in optoelectronic applications.
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