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Register a new userResonant photoluminescence and excitation spectroscopy of CdSe/ZnSe and CdTe/ZnTe self-assembled quantum dots
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Added by
Sebastian Mackowski
Publication date
2003
fields
Physics
and research's language is
English
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We show that two major carrier excitation mechanisms are present in II-VI self-assembled quantum dots. The first one is related to direct excited state - ground state transition. It manifests itself by the presence of sharp and intense lines in the excitation spectrum measured from single quantum dots. Apart from these lines, we also observe up to four much broader excitation lines. The energy spacing between these lines indicates that they are associated with absorption related to longitudinal optical phonons. By analyzing resonantly excited photoluminescence spectra, we are able to separate the contributions from these two mechanisms. In the case of CdTe dots, the excited state - ground state relaxation is important for all dots in ensemble, while phonon - assisted processes are dominant for the dots with smaller lateral size.
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Using micro- and nano-scale resonantly excited PL and PLE, we study the excitonic structure of CdSe/ZnSe and CdTe/ZnTe self assembled quantum dots (SAQD). Strong resonantly enhanced PL is seen at one to four optic phonon energies below the laser excitation energy. The maximum enhancement is not just one phonon energy above the peak energy distribution of QDs, but rather is 50 meV (for CdSe dots) or 100 meV (for CdTe) above the peak distribution. We interpret this unusual result as from double resonances associated with excited state to ground state energies being commensurate with LO phonons. Such a situation appears to occur only for the high-energy quantum dots.
We study the exciton spin relaxation in CdTe self-assembled quantum dots by using polarized photoluminescence spectroscopy in magnetic field. The experiments on single CdTe quantum dots and on large quantum dot ensembles show that by combining phonon-assisted absorption with circularly polarized resonant excitation the spin-polarized excitons are photo-excited directly into the ground states of quantum dots. We find that for single symmetric quantum dots at B=0 T, where the exciton levels are degenerate, the spins randomize very rapidly, so that no net spin polarization is observed. In contrast, when this degeneracy is lifted by applying external magnetic field, optically created spin-polarized excitons maintain their polarization on a time scale much longer than the exciton recombination time. We also observe that the exciton spin polarization is conserved when the splitting between exciton states is caused by quantum dot shape asymmetry. Similar behavior is found in a large ensemble of CdTe quantum dots. These results show that while exciton spins scatter rapidly between degenerate states, the spin relaxation time increases by orders of magnitude as the exciton spin states in a quantum dot become non-degenerate. Finally, due to strong electronic confinement in CdTe quantum dots, the large spin polarization of excitons shows no dependence on the number of phonons emitted between the virtual state and the exciton ground state during the excitation.
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.
The role of the sublimation of the compound and of the evaporation of the constituents from the gold nanoparticle during the growth of semiconductor nanowires is exemplified with CdTe-ZnTe heterostructures. Operating close to the upper temperature limit strongly reduces the amount of Cd present in the gold nanoparticle and the density of adatoms on the nanowire sidewalls. As a result, the growth rate is small and strongly temperature dependent, but a good control of the growth conditions allows the incorporation of quantum dots in nanowires with sharp interfaces and adjustable shape, and it minimizes the radial growth and the subsequent formation of additional CdTe clusters on the nanowire sidewalls, as confirmed by photoluminescence. Uncapped CdTe segments dissolve into the gold nanoparticle when interrupting the flux, giving rise to a bulb-like (pendant-droplet) shape attributed to the Kirkendall effect.
We present a comparative study of two self-assembled quantum dot (QD) systems based on II-VI compounds: CdTe/ZnTe and CdSe/ZnSe. Using magneto-optical techniques we investigated a large population of individual QDs. The systematic photoluminescence studies of emission lines related to the recombination of neutral exciton X, biexciton XX, and singly charged excitons (X$^+$, X$^-$) allowed us to determine average parameters describing CdTe QDs (CdSe QDs): X-XX transition energy difference 12 meV (24 meV); fine-structure splitting $delta_{1}=$0.14 meV ($delta_{1}=$0.47 meV); $g$-factor $g=$2.12 ($g=$1.71); diamagnetic shift $gamma=$2.5 $mu$eV$/$T$^{2}$ ($gamma=$1.3 $mu$eV$/$T$^{2}$). We find also statistically significant correlations between various parameters describing internal structure of excitonic complexes.
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