Ge microcrystals embedded in SiOZ glassy matrices were formed by a radio-frequency magnetron cosputtering technique and then annealed at 800 "C for 30 min. The average radius of the Ge microcrystals in SiOZ was determined to be about 3 nm by means of Raman spectroscopy and high resolution electron microscope. The annealed sample showed a strong room temperature luminescence with a peak at 2.18 eV. This is consistent with quantum confinement of electrons and holes.
The evolution of the optical phonon spectra of colloidal core/shell CdSe/ZnS quantum dots with an increase of the shell thickness from 0.5 to 3.4 monolayers has been studied by resonant Raman spectroscopy. The results obtained suggest that the ZnS shell changes its structure from amorphous to partly crystalline as the thickness increases. Simultaneously, an increase in Raman scattering by surface ͑core/shell interface͒ phonons and the redshift of the corresponding phonon band have been observed and assigned to variations in the shell structure. The disorder present in the shell provides a major contribution to the line shape of the Raman spectra at higher ZnS coverage. A method to control the quality of quantum dots based on Raman spectroscopy is proposed.
The photoluminescence (PL) spectra of CdSe-core CdS/CdZnS/ZnS-multishell quantum dots (QDs) were studied to understand the radiative and nonradiative relaxation processes in the temperature range from 80 to 360 K. The mechanism of temperature-dependent nonradiative relaxation processes in the CdSe QDs with changing the shell structures was found to evolve from thermal activation of carrier trapping by surface defects/traps in CdSe core QDs to the multiple longitudinal-optical (LO) phonon-assisted thermal escape of carriers in the core/shell QDs. An increase in PL intensity with increasing temperature was clearly observed in the core/shell QDs with a thick CdS monoshell and a CdS/ZnCdS/ZnS multishell. The PL enhancement was considered to come from delocalization of charge carriers localized at the CdSe/CdS interface with the potential depth of ∼30 meV. The experimental results indicated that the improvement of PL quantum efficiency in CdSe-core CdS/CdZnS/ZnS-multishell QDs could be understood in terms of the reduction of nonradiative recombination centers at the interfaces and on the surface of the multishell, as well as the confinement of electrons and holes into the QDs by an outer ZnS shell.
We have studied the electron spin relaxation in semiconductor InAs/GaAs quantum dots by time-resolved optical spectroscopy. The average spin polarization of the electrons in an ensemble of p-doped quantum dots decays down to 1/3 of its initial value with a characteristic time T(Delta) approximately 500 ps, which is attributed to the hyperfine interaction with randomly oriented nuclear spins. We show that this efficient electron spin relaxation mechanism can be suppressed by an external magnetic field as small as 100 mT.
We have studied the mechanism of photoluminescence (PL) from MnS/ZnS core/shell quantum dots (QDs) synthesized via hot solution phase chemistry using a nucleation-doping strategy. Efficient PL of the Mn 2+ ions with a quantum yield (QY) of over 35% is demonstrated in the resulting QDs coated with a thick ZnS shell on the MnS core. The MnS/ZnS core/shell QDs with a thick shell exhibit PL enhancement with increasing temperature in the range between 140 and 300 K, resulting from the thermal activation of charge carriers localized at the interface between the MnS core and the ZnS shell. The PL decays of the Mn 2+ ions in the core/shell QDs consist of three exponential components with time constants on the scales of 1-2 ms, hundreds of µs, and tens of µs. Surprisingly, the PL lifetimes of Mn 2+ ions show a very weak dependence on the shell thickness, which is clearly different from that of the PL QY of the QDs. The experimental results indicate that the mechanism for improving the PL QY in MnS/ZnS QDs can be understood in terms of a significantly enhanced energy transfer from the ZnS shell to Mn 2+ ions and a slightly decreased nonradiative relaxation rate from Mn 2+ ions to surface states/traps of the ZnS shell by the surface passivation of the QDs with a thick ZnS shell.
We present both theoretical and experimental investigations of optical properties of excitons in semiconductor-insulator quantum wires. Spectra of linear and nonlinear absorption, photoluminescence and its polarization, photoluminescence excitation, time-resolved photoluminescence of GaAs, CdSe, and InP quantum wires 4-6 nm in diameter, crystallized in dielectric matrix, demonstrate the prominent excitonic behavior. In these structures an essential difference of dielectric constants of constituent materials leads to a considerable enhancement of excitons, the binding energies ranging from 120 meV to 260 meV and exciton transitions being well distinguished in nanowires with sufficient dispersion of diameter even at room temperature. A theoretical approach to calculations of the exciton parameters in a semiconductor-insulator cylindrical quantum wire of finite diameter is developed. This approach accounts for a band-gap renormalization due to the spatial confinement and self-image effect, as well as for a dielectric enhancement of the electron-hole interaction. The calculated exciton transition energies and absorption spectra are consistent with the experimental results.
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