Resolving the emission transition dipole moments of single doubly-excited seeded nanorods via heralded defocused imaging

Semiconductor nanocrystal emission polarization is a crucial probe of nanocrystal physics and an essential factor for nanocrystal-based technologies. While the transition dipole moment of the lowest excited state to ground state transition is well characterized, the dipole moment of higher multiexcitonic transitions is inaccessible via most spectroscopy techniques. Here, we realize direct characterization of the doubly-excited state relaxation transition dipole by heralded defocused imaging. Defocused imaging maps the dipole emission pattern onto a fast single-photon avalanche diode detector array, allowing the post-selection of photon pairs emitted from the biexciton-exciton emission cascade and resolving the differences in transition dipole moments. Type-I1/2 seeded nanorods exhibit higher anisotropy of the biexciton-to-exciton transition compared to the exciton-to-ground state transition. In contrast, type-II seeded nanorods display a reduction of biexciton emission anisotropy. These findings are rationalized in terms of an interplay between transient dynamics of the refractive index and the excitonic fine structure

Two Biexciton Types Coexisting in Coupled Quantum Dot Molecules

Coupled colloidal quantum dot molecules (CQDMs) are an emerging class of nanomaterials, manifesting two coupled emission centers and thus introducing additional degrees of freedom for designing quantum-dot-based technologies. The properties of multiply excited states in these CQDMs are crucial to their performance as quantum light emitters, but they cannot be fully resolved by existing spectroscopic techniques. Here we study the characteristics of biexcitonic species, which represent a rich landscape of different configurations essentially categorized as either segregated or localized biexciton states. To this end, we introduce an extension of Heralded Spectroscopy to resolve the different biexciton species in the prototypical CdSe/CdS CQDM system. By comparing CQDMs with single quantum dots and with nonfused quantum dot pairs, we uncover the coexistence and interplay of two distinct biexciton species: A fast-decaying, strongly interacting biexciton species, analogous to biexcitons in single quantum dots, and a long-lived, weakly interacting species corresponding to two nearly independent excitons. The two biexciton types are consistent with numerical simulations, assigning the strongly interacting species to two excitons localized at one side of the quantum dot molecule and the weakly interacting species to excitons segregated to the two quantum dot molecule sides. This deeper understanding of multiply excited states in coupled quantum dot molecules can support the rational design of tunable single- or multiple-photon quantum emitters.U.B. and D.O. acknowledge the support of the Israel Science Foundation (ISF) and the Directorate for Defense Research and Development (DDR&D), grant No. 3415/21. J.I.C. and J.P. acknowledge support from UJI project B-2021-06. E.S., A.L., Y.E.P., and Y.O. acknowledge support from the Hebrew University Center for Nanoscience and Nanotechnology

Photon Correlations in Spectroscopy and Microscopy

Measurements of photon temporal correlations have been the mainstay of experiments in quantum optics. Over the past several decades, advancements in detector technologies have supported further extending photon correlation techniques to give rise to novel spectroscopy and imaging methods. This Perspective reviews the evolution of these techniques from temporal autocorrelations through multidimensional photon correlations to photon correlation imaging. State-of-the-art single-photon detector technologies are discussed, highlighting the main challenges and the unique current perspective of photon correlations to usher in a new generation of spectroscopy and imaging modalities.publishe

Quantum imaging with SPAD arrays

We present a novel quantum imaging modality based on photon correlation measurement with a single photon avalanche diode (SPAD) array in a confocal setup. This enables unprecedented simplicity in realization of photon correlation measurements, demonstrated via measuring of second and third order photon correlations of quantum light sources, and the implementation of a quantum based super-resolution technique

Quantum imaging with SPAD arrays (Conference Presentation)

The emerging field of quantum imaging introduces new methods to overcome classical limitations in optical microscopy. A detection apparatus capable of analyzing the quantum signature of light, is a crucial component in the heart of any such method. We present a novel quantum imaging modality, based on a state-of-the-art single photon avalanche diode (SPAD) array in a confocal setup. This modality enables unprecedented simplicity and scalability in imaging temporal photon correlations. We demonstrate the potential of this approach by measuring temporal correlations of classical and quantum sources, as well as demonstrate a quantum super-resolution technique