On-demand manipulation of superbunching emission from colloidal quantum dots and its application in noise-resistance correlated biphoton imaging

Abstract: Superbunching effect with second-order correlations larger than 2, $g^{(2)}(0)>2$, indicating the N-photon bundles emission and strong correlation among photons, has a broad range of fascinating applications in quantum illumination, communication, and computation. However, the on-demand manipulation of the superbunching effect in colloidal quantum dots (QDs) under pulsed excitation, which is beneficial to integrated photonics and lab-on-a-chip quantum devices, is still challenging. Here, we disclosed the evolution of $g^{(2)}(0)$ with the parameters of colloidal QDs by Mento Carlo simulations and performed second-order correlation measurements on CdSe/ZnS core/shell QDs under both continuous wave (CW) and pulsed lasers. The photon statistics of a single colloidal QD have been substantially tailored from sub-Poissonian distribution $g^{(2)}(0) <1$) to superbunching emission, with the maximum $g^{(2)}(0)$ reaching 69 and 20 under CW and pulsed excitation, respectively. We have achieved correlated biphoton imaging (CPI), employing the coincidence of the biexciton and bright exciton in one laser pulse, with the stray light and background noise up to 53 times stronger than PL emission of single colloidal QDs. By modulating the PL intensity, the Fourier-domain CPI with reasonably good contrast has been determined, with the stray light noise up to 107 times stronger than PL emission and 75600 times stronger than the counts of biphotons. Our noise-resistance CPI may enable laboratory-based quantum imaging to be applied to real-world applications with the highly desired suppression of strong background noise and stray light.