AI Article Synopsis
- Colloidal semiconductor nanocrystals, particularly giant CsPbBr nanocrystals, show promise for producing time-correlated and entangled photons through cascaded multiexcitonic emissions, despite challenges from nonradiative decay.
- The study demonstrates successful room-temperature spectroscopy of three-photon cascades from triexcitons, revealing strong correlation values that indicate weak binding of excitonic states.
- By analyzing fluorescence lifetimes and photon statistics, the researchers confirm emissions from higher multiexcitonic states and propose ways to control the statistics of emitted photons in future applications.
Article Abstract
Colloidal semiconductor nanocrystals have long been considered a promising source of time-correlated and entangled photons via the cascaded emission of multiexcitonic states. The spectroscopy of such cascaded emission, however, is hindered by efficient nonradiative Auger-Meitner decay, rendering multiexcitonic states nonemissive. Here we present room-temperature heralded spectroscopy of three-photon cascades from triexcitons in giant CsPbBr nanocrystals. We show that this system exhibits second- and third-order correlation function values, g(0) and g(0,0), close to unity, identifying very weak binding of both biexcitons and triexcitons. Combining fluorescence lifetime analysis, photon statistics, and spectroscopy, we can readily identify emission from higher multiexcitonic states. We use this to verify emission from a single emitter despite high emission quantum yields of multiply excited states and comparable emission lifetimes of singly and multiply excited states. Finally, we present potential pathways toward control of the photon number statistics of multiexcitonic emission cascades.
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| http://www.ncbi.nlm.nih.gov/pmc/articles/PMC11503816 | PMC |
| http://dx.doi.org/10.1021/acs.nanolett.4c03096 | DOI Listing |
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