Semiconductor nanocrystals feature multiply-excited states that display intriguing physics and significantly impact nanocrystal-based technologies. Fluorescence supplies a natural probe to investigate these states. Still, direct observation of multiexciton fluorescence has proved elusive to existing spectroscopy techniques. Heralded Spectroscopy is a new tool based on a breakthrough single-particle, single-photon, sub-nanosecond spectrometer that utilizes temporal photon correlations to isolate multiexciton emission. This proceedings paper introduces Heralded Spectroscopy and reviews some of the novel insights it uncovered into exciton–exciton interactions within single nanocrystals. These include weak exciton–exciton interactions and their correlation with quantum confinement, biexciton spectral diffusion, multiple biexciton species and biexciton emission polarization.
Since the introduction of the intensity interferometer by Hanbury Brown and Twiss in the '50s and its subsequent adaptations to quantum optic experiments, photon correlations have played a significant role in optical research. An emerging detector technology, SPAD arrays, presents new opportunities to scale these experiments and exploit photon correlations in new regimes. I will describe a new temporal-spectral photon correlation technique based on these detectors, single-particle heralded spectroscopy. I will present new insights into the photophysics of multiply-excited semiconductor quantum dots uncovered by this method, hitherto inaccessible to existing approaches.
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