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Register a new userRadiative recombination of charged excitons and multiexcitons in CdSe quantum dots
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Added by
Claudia Troparevsky
Publication date
2005
fields
Physics
and research's language is
English
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We report semi-empirical pseudopotential calculations of emission spectra of charged excitons and biexcitons in CdSe nanocrystals. We find that the main emission peak of charged multiexcitons - originating from the recombination of an electron in an s-like state with a hole in an s-like state - is blue shifted with respect to the neutral mono exciton. In the case of the negatively charged biexciton, we observe additional emission peaks of lower intensity at higher energy, which we attribute to the recombination of an electron in a p state with a hole in a p state.
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We study spin dynamics of excitons confined in self-assembled CdSe quantum dots by means of optical orientation in magnetic field. At zero field the exciton emission from QDs populated via LO phonon-assisted absorption shows a circular polarization of 14%. The polarization degree of the excitonic emission increases dramatically when a magnetic field is applied. Using a simple model, we extract the exciton spin relaxation times of 100 ps and 2.2 ns in the absence and presence of magnetic field, respectively. With increasing temperature the polarization of the QD emission gradually decreases. Remarkably, the activation energy which describes this decay is independent of the external magnetic field, and, therefore, of the degeneracy of the exciton levels in QDs. This observation implies that the temperature-induced enhancement of the exciton spin relaxation is insensitive to the energy level degeneracy and can be attributed to the same excited state distribution.
We present results on the charge dependence of the radiative recombination lifetime, Tau, and the emission energy of excitons confined to single self-assembled InGaAs quantum dots. There are significant dot-to-dot fluctuations in the lifetimes for a particular emission energy. To reach general conclusions, we present the statistical behavior by analyzing data recorded on a large number of individual quantum dots. Exciton charge is controlled with extremely high fidelity through an n-type field effect structure, providing access to the neutral exciton (X0), the biexciton (2X0) and the positively (X1+) and negatively (X1-) charged excitons. We find significant differences in the recombination lifetime of each exciton such that, on average, Tau(X1-) / Tau(X0) = 1.25, Tau(X1+) / Tau(X0) = 1.58 and Tau(2X0) / Tau(X0) = 0.65. We attribute the change in lifetime to significant changes in the single particle hole wave function on charging the dot, an effect more pronounced on charging X0 with a single hole than with a single electron. We verify this interpretation by recasting the experimental data on exciton energies in terms of Coulomb energies. We show directly that the electron-hole Coulomb energy is charge dependent, reducing in value by 5-10% in the presence of an additional electron, and that the electron-electron and hole-hole Coulomb energies are almost equal.
We measured, for the first time, two photon radiative cascades due to sequential recombination of quantum dot confined electron hole pairs in the presence of an additional spectator charge carrier. We identified direct, all optical cascades involving spin blockaded intermediate states, and indirect cascades, in which non radiative relaxation precedes the second recombination. Our measurements provide also spin dephasing rates of confined carriers.
We have used the variable stripe technique and pump-probe spectroscopy to investigate both gain and the dynamics of amplified spontaneous emission from CdSe quantum dot structures. We have found modal gain coefficients of 75 and 32 1/cm for asymmetric and symmetric waveguide structures, respectively. Amplified spontaneous emission decay times of 150 and 300 ps and carrier capture times of 15 and 40 ps were measured for the structures with high and low material gains respectively. The difference in the capture times are related to the fact that for the symmetric waveguide, carriers diffuse into the active region from the uppermost ZnMgSSe cladding layer, yielding a longer rise time for the pump-probe signals for this sample.
We report on polarization-resolved resonant photoluminescence (PL) spectroscopy of bright (spin-1) and dark (spin-2) excitons in colloidal CdSe nanocrystal quantum dots. Using high magnetic fields to 33 T, we resonantly excite (and selectively analyze PL from) spin-up or spin-down excitons. At low temperatures (<4K) and above ~10 T, the spectra develop a narrow, circularly polarized peak due to spin-flipped bright excitons. Its evolution with magnetic field directly reveals a large (1-2 meV), intrinsic fine structure splitting of bright excitons, due to anisotropic exchange. These findings are supported by time-resolved PL studies and polarization-resolved PL from single nanocrystals.
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