We report circular-to-linear and linear-to-circular conversion of optical polarization by semiconductor quantum dots. The polarization conversion occurs under continuous wave excitation in the absence of any magnetic field. The effect originates from quantum interference of linearly and circularly polarized photon states, induced by the natural anisotropic shape of the self-assembled dots. The behavior can be qualitatively explained in terms of a pseudospin formalism.
We study the dynamics of photoexcited electrons and holes in single negatively charged CdSe/ZnSe quantum dots with two-color femtosecond pump-probe spectroscopy. An initial characterization of the energy level structure is performed at low temperatures and magnetic fields of up to 5 T. Emission and absorption resonances are assigned to specific transitions between few-fermion states by a theoretical model based on a configuration interaction approach. To analyze the dynamics of individual charge carriers, we initialize the quantum system into excited trion states with defined energy and spin. Subsequently, the time-dependent occupation of the trion ground state is monitored by spectrally resolved differential transmission measurements. We observe subpicosecond dynamics for a hole excited to the D shell. The energy dependence of this D-to-S shell intraband transition is investigated in quantum dots of varying size. Excitation of an electron-hole pair in the respective p shells leads to the formation of singlet and triplet spin configurations. Relaxation of the p-shell singlet is observed to occur on a time scale of a few picoseconds. Pumping of p-shell triplet transitions opens up two pathways with distinctly different scattering times. These processes are shown to be governed by the mixing of singlet and triplet states due to exchange interactions enabling simultaneous electron and hole spin flips. To isolate the relaxation channels, we align the spin of the residual electron by a magnetic field and employ laser pulses of defined helicity. This step provides ultrafast preparation of a fully inverted trion ground state of the quantum dot with near unity probability, enabling deterministic addition of a single photon to the probe pulse. Therefore our experiments represent a significant step towards using single quantum emitters with well-controled inversion to manipulate the photon statistics of ultrafast light pulses.
We report a systematic study of magneto-optical properties in CdZnSe/ZnSe semiconductor quantum dots ͑QDs͒ subjected to postgrowth thermal annealing. The theoretical and experimental characterizations are combined in order to understand the evolution of Zeeman splitting and the blueshift as well as redshift of the magnetic subcomponents with magnetic field strength of excitons confined in annealed QDs as a function of different annealing times. A combination of a multiband model as well as parameter interpolation supported by ab initio calculations is presented and points toward an inversion of the light-hole-heavy-hole states due to annealing. The band mixing of exciton states explains besides the variation in the Zeeman splitting for differently annealed QD excitons, the evolution of the diamagnetic blueshift into a paramagnetic redshift of the magnetic subcomponents. A discussion of the effects associated to the Coulomb interaction on the polarized excitonic recombinations modulated by magnetic field is given.
We report on a complex nontrivial behavior of the optical anisotropy of quantum dots that is induced by a magnetic field in the plane of the sample. We find that the optical axis either rotates in the opposite direction to that of the magnetic field or remains fixed to a given crystalline direction. A theoretical analysis based on the exciton pseudospin Hamiltonian unambiguously demonstrates that these effects are induced by isotropic and anisotropic contributions to the heavy-hole Zeeman term, respectively. The latter is shown to be compensated by a built-in uniaxial anisotropy in a magnetic field BC = 0.4 T, resulting in an optical response typical for symmetric quantum dots.
The formation of CdSe/ZnSe quantum dots by a method combining a low temperature MBE growth of a CdSe layer and its subsequent in-situ annealing at temperatures between 280−340• C has been studied. The thermal treatment results in a re-organization of the surface from a nearly two--dimensional layer to an ensemble of three-dimensional dot-like features. In this work we optimized the different growth and annealing parameters of this process and compared the properties of the resultant dots with those of dots grown by conventional MBE at 300• C. It is demonstrated that the luminescence properties of the dots for both growth techniques are comparable but the areal density achieved by the in-situ annealing technique is an order of magnitude lower. From high resolution X-ray diffraction results, it could be established that no desorption takes place despite significantly long annealing duration. Beyond a nominal coverage of 3.5 ML CdSe, stacking faults are generated, leading to a gradual decrease in luminescence intensities and an overlap of pendellösung fringes in X-ray diffractograms.
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