arXiv subjects
Publications and source records attributed to L. M. Smith.
We use spatially resolved micro-PL imaging at low temperature to study optical properties of two sets of CdS nanowires grown using 20 nm and 50 nm catalysts. We find that low temperature PL of single nanowires is an ideal technique to gauge the quality of a given growth run, and moreover enables the collection of detailed spatial information on single wire electronic states.
We study the optical properties of a single core-shell GaAs-AlGaAs nanowire (grown by VLS method) using the technique of micro-photoluminescence and spatially-resolved photoluminescence imaging. We observe large linear polarization anisotropy in emission and excitation of nanowires.
Time-resolved photoluminescence (PL) and micro-PL imaging were used to study single CdS nanowires at 10 K. The low-temperature PL of all CdS nanowires exhibit spectral features near energies associated with free and bound exciton transitions, with the transition energies and emission intensities varying along the length of the nanowire. In addition, several nanowires show spatially localized PL at lower energies which are associated with morphological irregularities in the nanowires. Time-resolved PL measurements indicate that exciton recombination in all CdS nanowires is dominated by non-radiative recombination at the surface of the nanowires.
Temperature dependent photoluminescence (PL) is used to study the electronic properties of single CdS nanowires. At low temperatures, both near-band edge (NBE) photoluminescence (PL) and spatially-localized defect-related PL are observed in many nanowires. The intensity of the defect states is a sensitive tool to judge the character and structural uniformity of nanowires. As the temperature is raised, the defect states rapidly quench at varying rates leaving the NBE PL which dominates up to room temperature. All PL lines from nanowires follow closely the temperature-dependent band edge, similar to that observed in bulk CdS.
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 observe a strong dependence of the exciton spin relaxation in CdTe quantum dots on the average dot size and the depth of the confining potential. For the excitons confined to the as-grown CdTe quantum dots we find the spin relaxation time to be 4.8 ns. After rapid thermal annealing, which increases the average dot size and leads to weaker confinement, we measure the spin relaxation tine to be 1.5 ns, resulting in smaller values of the absolute polarization of the quantum dot emission. This dramatic enhancement of the spin scattering efficiency upon annealing is attributed to increased mixing between different spin states in larger CdTe quantum dots.
We show that through the resonant optical excitation of spin-polarized excitons into CdMnTe magnetic quantum dots, we can induce a macroscopic magnetization of the Mn impurities. We observe very broad (4 meV linewidth) emission lines of single dots, which are consistent with the formation of strongly confined exciton magnetic polarons. Therefore we attribute the optically induced magnetization of the magnetic dots results to the formation of spin-polarized exciton magnetic polarons. We find that the photo-induced magnetization of magnetic polarons is weaker for larger dots which emit at lower energies within the QD distribution. We also show that the photo-induced magnetization is stronger for quantum dots with lower Mn concentration, which we ascribe to weaker Mn-Mn interaction between the nearest neighbors within the dots. Due to particular stability of the exciton magnetic polarons in QDs, where the localization of the electrons and holes is comparable to the magnetic exchange interaction, this optically induced spin alignment persists to temperatures as high as 160 K.
We demonstrate sub-wavelength imaging of excitons confined to single CdTe quantum dots. By combining slit-confocal microscopy with a hemispherical solid immersion lens we simultaneously map the emission of thousands of single quantum dots with a spatial resolution of 400 nm. By analyzing the linear polarization of the quantum dot emissions at B=0T, we find that the distribution of the exchange splitting is centered at zero with a standard deviation of 0.34 meV. Similar experiments performed at B=3T give an average value of the exciton effective g factor of 3.1. This experimental approach provides an effective means to gain statistical information about the quantum dot exciton fine structure in the ensemble.
We demonstrate that resonant excitation of CdMnTe self-assembled quantum dots creates an ensemble of spin-polarized magnetic polarons at B=0 T. The strong spatial confinement characteristic of quantum dots significantly increases the stability of magnetic polarons so that the optically induced spin alignment is observed for temperatures > 120 K.
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.
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.
Using resonantly excited photoluminescence along with photoluminescence excitation spectroscopies, we study the carrier excitation processes in CdTe/ZnTe and CdSe/ZnSe self-assembled quantum dots. Photoluminescence excitation spectra of single CdTe quantum dots reflect two major mechanisms for carrier excitation: The first, associated with the presence of sharp and intense lines in the spectrum, is a direct excited state ? ground state transition. The second, associated with the appearance of up to four much broader excitation lines, is a LO phonon-assisted absorption directly into the quantum dot ground states. LO phonons with energies of both quantum dots and ZnTe barrier material are identified in the photoluminescence excitation spectra. Resonantly excited PL measurements for the dot ensemble as a function of excitation energy makes it possible to separate the contributions of these two mechanisms. We find that for CdTe quantum dots the distribution of excited states coupled to the ground states reflects the energy distribution of the quantum dot emission, but shifted up in energy by 100 meV. This large splitting between excited and ground states in CdTe quantum dots suggests strong spatial confinement. In contrast, the LO phonon-assisted absorption shows significant size selectivity. In the case of CdTe dots the exciton-LO phonon coupling is strongly enhanced for smaller-sized dots which have higher emission energies. In contrast, for CdSe quantum dots the exciton-LO phonon coupling is uniform over the ensemble ? that is, the energy distribution determines the intensities of LO phonon replicas. We show that for CdTe quantum dots after annealing, that is after an increase in the average dot size, the exciton-LO phonon interaction reflects the dot energy distribution, as observed for CdSe quantum dots.
We study the excitonic structure of CdSe/ZnSe self assembled quantum dots (SAQD) by magneto-photoluminescence (PL) spectroscopy. Using fixed 200 nm apertures through a metal film, we are able to probe single narrow (200 micro-eV) spectroscopic lines emitted from CdSe quantum dots at 2K. Using linear polarization analysis of these lines, we find that approximately half of the quantum dots are elliptically elongated along the [110] direction. The other half of the QDs are symmetric, with emission lines which are completely unpolarized at zero field and exhibit no doublet structure. Using an applied magnetic field, we obtain the diamagnetic shift and the g-factor for several symmetric dots and find that the variation from dot to dot is random, with no systematic dependence with emission energy. In addition, we find no correlation between the diamagnetic shift and the g-factor.
We show that CdMnTe self-assembled quantum dots can be formed by depositing a submonolayer of Mn ions over a ZnTe surface prior to deposition of the CdTe dot layer. Single dot emission lines and strongly polarized quantum dot photoluminescence in an applied magnetic field confirm the presence of Mn in individual quantum dots. The width of PL lines of the single CdMnTe dots is 3 meV due to magnetic moment fluctuations of the Mn ions. After rapid thermal annealing, the emission lines of individual magnetic quantum dots narrow significantly to 0.25 meV showing that effect of magnetic fluctuations is strongly reduced most probably due to an increase in the average quantum dot size. These results suggest a way to tune the spin properties of magnetic quantum dots.
We demonstrate a new method of measuring the exciton spin relaxation time in semiconductor nanostructures by continuous-wave photoluminescence. We find that for self-assembled CdTe quantum dots the degree of circular polarization of emission is larger when exciting polarized excitons into the lower energy spin state than in the case when the excitons are excited into the higher energy spin state. A simple rate equation model gives the exciton spin relaxation time in CdTe quantum dots equal to 4.8+/-0.3 ns, significantly longer than the quantum dot exciton recombination time 300 ps.
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.