Strong Purcell effect observed in single thick shell CdSe/CdS nanocrystals coupled to localized surface plasmons

High quality factor dielectric cavities designed to a nanoscale accuracy are mostly used to increase the spontaneous emission rate of a single emitter. Here we show that the coupling, at room temperature, between thick shell CdSe/CdS nanocrystals and random metallic films offers a very promising alternative approach. Optical modes confined at the nanoscale induce strong Purcell factors reaching values as high as 60. Moreover the quantum emission properties can be tailored: strong antibunching or radiative biexcitonic cascades can be obtained with high photon collection efficiency and extremely reduced blinking.Comment: 16 pages, 7 figure

Hyperfine Interactions and Slow Spin Dynamics in Quasi-isotropic InP-based Core/Shell Colloidal Nanocrystals

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Blinking suppression and biexcitonic emission in thick-shell CdSe/CdS nanocrystals at cryogenic temperature

International audienceThe fluorescence of single colloidal thick-shell CdSe/CdS nanocrystals (NCs), at cryogenic temperature (4 K) and room temperature (RT), is studied using the intensity autocorrelation function (ACF) and lifetime measurements. The radiative and Auger decay rates corresponding to the desexcitation of the charged biexcitonic state are determined through an original method of photon postselection. Especially, the charged biexciton quantum yield increases from about 15% at RT to 60% at 4 K. The high inhibition of Auger recombination already observed for the trion state of CdSe/CdS NCs at low temperature is also demonstrated for the charged biexcitonic state. At 4 K, the ACF is equal to 1 for time scales ranging from 50 ns to 200 ms. In contrast with RT operation, the intensity of the trion emission is then perfectly stable and no blinking is observed. All the results highlight the strong confinement of the charge carriers in the CdSe core

Negatively charged and dark excitons in CsBbBr3 perovskite nanocrystals revealed by high magnetic fields

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Hyperfine Interactions and Slow Spin Dynamics in Quasi-isotropic InP-based Core/Shell Colloidal Nanocrystals

Colloidal InP core nanocrystals are taking over CdSe-based nanocrystals, notably in optoelectronic applications. Despite their use in commercial devices, such as display screens, the optical properties of InP nanocrystals and especially their relation to the exciton fine structures remain poorly understood. In this work, we show that the ensemble magneto-optical properties of InP-based core/shell nanocrystals investigated in strong magnetic fields up to 30 T are strikingly different from other colloidal nanostructures. Notably, the mixing of the lowest spin-forbidden dark exciton state with the nearest spin-allowed bright state does not occur up to the highest magnetic fields applied. This lack of mixing in an ensemble of nanocrystals suggests an anisotropy tolerance of InP nanocrystals. This striking property allowed us to unveil the slow spin dynamics between Zeeman sublevels (up to 400 ns at 15 T). Furthermore, we show that the unexpected magnetic-field-induced lengthening of the dark exciton lifetime results from the hyperfine interaction between the spin of the electron in the dark exciton with the nuclear magnetic moments. Our results demonstrate the richness of the spin physics in InP quantum dots and stress the large potential of InP nanostructures for spin-based applications

Trap-free heterostructure of PbS nanoplatelets on InP(001) by chemical epitaxy

International audienceSemiconductor nanocrystalline heterostructures can be produced by the immersion of semiconductor substrates into an aqueous precursor solution, but this approach usually leads to a high density of interfacial traps. In this work, we study the effect of a chemical passivation of the substrate prior to the nanocrystalline growth. PbS nanoplatelets grown on sulfur-treated InP (001) surfaces at temperatures as low as 95 °C exhibit abrupt crystalline interfaces that allow a direct and reproducible electron transfer to the InP substrate through the nanometer-thick nanoplatelets with scanning tunnelling spectroscopy. It is in sharp contrast with the less defined interface and the hysteresis of the current–voltage characteristics found without the passivation step. Based on a tunnelling effect occurring at energies below the bandgap of PbS, we show the formation of a type II, trap-free, epitaxial heterointerface, with a quality comparable to that grown on a nonreactive InP (110) substrate by molecular beam epitaxy. Our scheme offers an attractive alternative to the fabrication of semiconductor heterostructures in the gas phase

Hyperfine interactions and slow spin dynamics in quasi-isotropic InP-based core/shell colloidal nanocrystals

Colloidal InP core nanocrystals are taking over CdSe-based nanocrystals, notably in optoelectronic applications. Despite their use in commercial devices, such as display screens, the optical properties of InP nanocrystals and especially their relation to the exciton fine structures remain poorly understood. In this work, we show that the ensemble magneto-optical properties of InP-based core/shell nanocrystals investigated in strong magnetic fields up to 30 T are strikingly different from other colloidal nanostructures. Notably, the mixing of the lowest spin-forbidden dark exciton state with the nearest spin-allowed bright state does not occur up to the highest magnetic fields applied. This lack of mixing in an ensemble of nanocrystals suggests an anisotropy tolerance of InP nanocrystals. This striking property allowed us to unveil the slow spin dynamics between Zeeman sublevels (up to 400 ns at 15 T). Furthermore, we show that the unexpected magnetic-field-induced lengthening of the dark exciton lifetime results from the hyperfine interaction between the spin of the electron in the dark exciton with the nuclear magnetic moments. Our results demonstrate the richness of the spin physics in InP quantum dots and stress the large potential of InP nanostructures for spin-based applications