Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.278
Publication date: 16th December 2024
Colloidal perovskite nanocrystals have emerged as promising candidates for next-generation quantum light sources based on their excellent optical properties. In this context, the method to optically prepare the emitting states is a critical step. While previous works on epitaxial quantum dots have stablished that resonant excitation can improve the performance of quantum emitter when compared to above-bandgap excitation by avoid the dephasing processes involved in hot carrier cooling, low-background resonant excitation of a single colloidal perovskite nanocrystal has not yet been achieved. Here, we demonstrate resonant three-photon excitation (3PE) of a single perovskite nanorod at both room temperature and cryogenic temperature. Third-harmonic generation, arising as a background created from the substrate interface is observed and further eliminated using polarization by a factor of 105, resulting in a signal to background ratio larger than 100. The giant three-photon absorption cross-section at room temperature is measured to be around 10-76 cm6·s2·photon-2 at resonance, which is two orders of magnitude larger than those of traditional CdSe-based nanocrystals. Additionally, similar fluorescence and blinking properties between upper-bandgap 1PE and resonant 3PE are observed in room temperature, highlighting the sample’s photostability under high power NIR beams. This low-background resonant three-photon excitation method has great potential to improve the optical coherence properties of perovskite nanocrystal.
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