ArticleACS nano2026
Vanishing Quantum Confinement Enables Bright and Thermally Excited Multicarrier Emission from Semiconductor Nanocrystals.
Article in ACS nano, 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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Abstract
Recently, nanocrystals in the regime of vanishing quantum confinement─termed bulk nanocrystals (BNCs)─have demonstrated optical gain characteristics. While their high-power lasing performance was demonstrated convincingly, the photophysics at low and intermediate powers─where charge-carrier populations are discrete─remain unexplored. Using single-photon avalanche diode (SPAD) array technology, we resolve the dynamics and energetics of six multicarrier excited states in individual CdSe/CdS core/shell BNCs, containing up to four electrons and two holes. Each state exhibits bimodal emission, indicative of thermal equilibrium between closely spaced electron and hole levels, confirmed via temperature-dependent single-particle measurements. Quantification of radiative and nonradiative decay channels reveals strongly suppressed Auger recombination through both the negative- and positive-trion pathways. We present a model that combines statistical scaling of rate constants with Fermi-Dirac thermal occupations of electron and hole levels, bridging the transitional regime between quantum-confined and bulk nanocrystals, and providing a comprehensive framework for understanding this emerging class of materials.
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