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Higher-order nonclassicality for clusters of single-photon emitters

Qi Luo, Mathieu Manceau, Andrea Cavanna, Fabian Gumpert, Luigi Carbone, Massimo De Vittorio, Alberto Bramati, E. Giacobino, Maria V. Chekhova

Published Jan 28, 2018• 1 citation
OpenAlex

Abstract

We consider nonclassical features of light emitted by clusters of room-temperature single-photon emitters. As signatures of nonclassicality, we discuss violation of inequalities for normalized correlation functions of orders higher than two. These conditions are stronger than higher-order antibunching, i.e., higher-order normalized correlation functions being less than unity. In experiment, we observe third-order nonclassicality as well as second-, third-, and fourth-order antibunching for clusters of 1 to 20 colloidal CdSe/CdS dot-in-rods.

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Optics Letters•Dec 1, 2001•160 citations
We consider nonclassical features of light emitted by clusters of room-temperature single-photon emitters. As signatures of nonclassicality, we discuss violation of inequalities for normalized correlation functions of orders higher than two. These conditions are stronger than higher-order antibunching, i.e., higher-order normalized correlation functions being less than unity. In experiment, we observe third-order nonclassicality as well as second-, third-, and fourth-order antibunching for clusters of 1 to 20 colloidal CdSe/CdS dot-in-rods.
We study nonclassical features of multiphoton light emitted by clusters of single-photon emitters. As signatures of nonclassicality, we use violation of inequalities for normalized correlation functions of different orders or the probabilities of multiphoton detection. In particular, for clusters of 2–14 colloidal CdSe/CdS dot-in-rods we observe antibunching and nonclassicality of up to the fourth-order. Surprisingly, violation of certain classical inequalities gets even more pronounced for larger clusters.
Images of semiconductor "dot-in-rods" and their small clusters are studied by measuring the second-order correlation function with a spatially resolving intensified CCD camera. This measurement allows one to distinguish between a single dot and a cluster and, to a certain extent, to estimate the number of dots in a cluster. A more advanced measurement is proposed, based on higher-order correlations, enabling more accurate determination of the number of dots in a small cluster. Nonclassical features of the light emitted by such a cluster are analyzed.
Images of semiconductor "dot-in-rods" and their small clusters are studied by measuring the second-order correlation function with a spatially resolving intensified CCD camera. This measurement allows one to distinguish between a single dot and a cluster and, to a certain extent, to estimate the number of dots in a cluster. A more advanced measurement is proposed, based on higher-order correlations, enabling more accurate determination of the number of dots in a small cluster. Nonclassical features of the light emitted by such a cluster are analyzed.
In this thesis, an experiment for testing the non-classicality of the light emitted by CdSe/CdS clusters is described. Different criteria are used, which are sufficient conditions for the non-classicality. They are based on the measurement of normalized Glauber’s correlation functions of different orders or multi-photon probabilities using the Hanbury Brown–Twiss (HBT) setup. After measuring the light emitted by CdSe/CdS clusters consisting of different numbers of quantum dots, the non-classicality of their emission has been verified with using the criteria mentioned above. In particular, the fourth-order anti-bunching and the non-classicality witnessed by the Klyshko criteria of the third-order have been observed in this experiment, which have never been reported on a triggered multi-photon source before, to the best of my knowledge. In this thesis, an experiment of calibrating the QE of the intensified CCD (ICCD) camera in the single-photon detection regime with using Klyshko’s absolute method has been described. Different groups of pixels in the same camera have been used as both the reference and calibrated detectors, and therefore this is an autonomous absolute calibration. The QE of the ICCD camera as a function of the threshold value, as well as the wavelength dependence of the QE at a chosen threshold value, have been measured. The QE value in the single-photon regime is much lower than the one of the photocathode of the camera. To the best of my knowledge, this is the first experiment to calibrate the QE of an ICCD camera in the single-photon regime. The experimental results reported in this thesis are useful in the field of non-classical multi-photon sources as well as the field of multiplexed single-photon detection techniques.
We use the third- and fourth-order autocorrelation functions ${g}^{(3)}({\ensuremath{\tau}}_{1},{\ensuremath{\tau}}_{2})$ and ${g}^{(4)}({\ensuremath{\tau}}_{1},{\ensuremath{\tau}}_{2},{\ensuremath{\tau}}_{3})$ to detect the nonclassical character of the light transmitted through a photonic-crystal nanocavity containing a strongly coupled quantum dot probed with a train of coherent light pulses. We contrast the value of g(3)(0,0){g}^{(3)}(0,0)g(3)(0,0) with the conventionally used g(2)(0){g}^{(2)}(0)g(2)(0) and demonstrate that, in addition to being necessary for detecting two-photon states emitted by a low-intensity source, g(3){g}^{(3)}g(3) provides a more clear indication of the nonclassical character of a light source. We also present preliminary data that demonstrates bunching in the fourth-order autocorrelation function ${g}^{(4)}({\ensuremath{\tau}}_{1},{\ensuremath{\tau}}_{2},{\ensuremath{\tau}}_{3})$ as the first step toward detecting three-photon states.
The fluorescence of single-colloidal CdSe quantum dots is investigated at room temperature by means of the autocorrelation function over a time scale of almost 12 orders of magnitude. Over a short time scale, the autocorrelation function shows complete antibunching, indicating single-photon emission and atomiclike behavior. Over longer time scales (up to tens of seconds), we measure a bunching effect that is due to fluorescence intermittency and that cannot be described by fluctuations between two states with constant rates. The autocorrelation function also exhibits nonstationary behavior related to power-law distributions of On and Off times.