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The unusual temperature dependence of exciton emission decay in CsPbX3 perovskite nanocrystals (NCs) attracts considerable attention. Upon cooling, extremely short (sub-ns) lifetimes were observed and were explained by an inverted bright-dark state splitting. Here, we report temperature-dependent exciton lifetimes for CsPbCl3 NCs doped with 0-41% Mn2+. The exciton emission lifetime increases upon cooling from 300 to 75 K. Upon further cooling, a strong and fast sub-ns decay component develops. However, the decay is strongly biexponential and also a weak, slow decay component is observed with a ∼40-50 ns lifetime below 20 K. The slow component has a ∼5-10 times stronger relative intensity in Mn-doped NCs compared to that in undoped CsPbCl3 NCs. The temperature dependence of the slow component resembles that of CdSe and PbSe quantum dots with an activation energy of ∼19 meV for the dark-bright state splitting. Based on our observations, we propose an alternative explanation for the short, sub-ns exciton decay time in CsPbX3 NCs. Slow bright-dark state relaxation at cryogenic temperatures gives rise to almost exclusively bright state emission. Incorporation of Mn2+ or high magnetic fields enhances the bright-dark state relaxation and allows for the observation of the long-lived dark state emission at cryogenic temperatures.
citations This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically). | 65 | |
popularity This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network. | Top 1% | |
influence This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically). | Top 10% | |
impulse This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network. | Top 10% |