Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.032
Publication date: 18th July 2023
The advent of SPAD-array based parallelized detection of time-stamped single photons opens a pathway for extracting previously inaccessible spectroscopic information from dim sources of quantum light. In particular, it enables to multiplex detection both in time and in additional dimensions such as space, frequency or spatial frequency. We use this to study the interactions between pairs of excitons in doubly excited colloidal semiconductor nanocrystals, revealing weak multielectron effects at room temperature against a strong temperature broadened background.
We present heralded spectroscopy [1], the unique identification and post-selection of pair emission events from single nanocrystals while performing a spectral measurement (using a line SPAD array [1]) or a defocused imaging measurement (using a 2D SPAD array [2]). Using this method we can characterize subtle differences between the first emitted photon (representing emission from the doubly excited state) and the second emitted photon (representing the singly excited state). Several examples for this will be given, including interaction effects on emission anisotropy from semiconductor nanorods [2] and identification of multiexcitonic states in quantum dot molecules. The utility of our method for study of higher excited states via three-photon correlation will also be discussed.
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