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Register a new userCdSe/CdS dot-in-rods nanocrystals fast blinking dynamics
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The blinking dynamics of colloidal core-shell CdSe/CdS dot-in-rods is studied in detail at the single particle level. Analyzing the autocorrelation function of the fluorescence intensity, we demonstrate that these nanoemitters are characterized by a short value of the mean duration of bright periods (ten to a few hundreds of microseconds). The comparison of the results obtained for samples with different geometries shows that not only the shell thickness is crucial but also the shape of the dot- in-rods. Increasing the shell aspect ratio results in shorter bright periods suggesting that surface traps impact the stability of the fluorescence intensity.
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The photon statistics of CdSe/CdS dot-in-rods nanocrystals is studied with a method involving post-selection of the photon detection events based on the photoluminescence count rate. We show that flickering between two states needs to be taken into account to interpret the single-photon emission properties. With post-selection we are able to identify two emitting states: the exciton and the charged exciton (trion), characterized by different lifetimes and different second order correlation functions. Measurements of the second order autocorrelation function at zero delay with post- selection shows a degradation of the single photon emission for CdSe/CdS dot-in-rods in a charged state that we explain by deriving the neutral and charged biexciton quantum yields.
We prove experimentally, upon polarization analysis performed on a large statistic of single nanoemitters, that high quality core/shell CdSe/CdS dot-in-rods behave as linear dipoles. Moreover, the dipole in-plane and out-of-plane orientations could be assessed. We demonstrate in particular that, contrary to expectations, the emitting dipole is not aligned with the elongated axis of the dot-in-rod. Besides, the polarimetric measurements prove that the excitation transition cannot be approximated by a single linear dipole, contrary to the emission transition. Finally, we highlight that non-radiative channels of charge carrier recombination do not affect the dipolar nature of the radiative transitions.
The photoluminescence intermittency (blinking) of quantum dots is interesting because it is an easily-measured quantum process whose transition statistics cannot be explained by Fermis Golden Rule. Commonly, the transition statistics are power-law distributed, implying that quantum dots possess at least trivial memories. By investigating the temporal correlations in the blinking data, we demonstrate with high statistical confidence that quantum dot blinking data has non-trivial memory, which we define to be statistical complexity greater than one. We show that this memory cannot be discovered using the transition distribution. We show by simulation that this memory does not arise from standard data manipulations. Finally, we conclude that at least three physical mechanisms can explain the measured non-trivial memory: 1) Storage of state information in the chemical structure of a quantum dot; 2) The existence of more than two intensity levels in a quantum dot; and 3) The overlap in the intensity distributions of the quantum dot states, which arises from fundamental photon statistics.
Although poorly understood, cation-exchange reactions are increasingly used to dope or transform colloidal semiconductor nanocrystals (quantum dots). We used density-functional theory and kinetic Monte Carlo simulations to develop a microscopic theory that explains structural, optical, and electronic changes observed experimentally in Ag-cation-exchanged CdSe nanocrystals. We find that Coulomb interactions, both between ionized impurities and with the polarized nanocrystal surface, play a key role in cation exchange. Our theory also resolves several experimental puzzles related to photoluminescence and electrical behavior in CdSe nanocrystals doped with Ag.
We study the electronic properties of spherical quantum dot quantum well nanocrystals within a symmetry-based tight-binding model. In particular, the influence of a concentric monolayer of HgS embedded in a spherical CdS nanocrystal of diameter 52.7 A is analyzed as a function of its distance from the center. The electron and hole states around the energy gap show a strong localization in the HgS well and the neighboring inner (core) interface region. Important effects on the optical properties such as the absorption gap and the fine structure of the exciton spectrum are also reported.
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