Surface modification of Co-doped ZnO nanocrystals and its effects on the magnetic properties

A series of chemically prepared Co2+-doped ZnO colloids has been surface modified either by growing shells of ZnSe or by the in situ encapsulation in poly styrene . The surface modification effects using these two distinct chemical strategies on the magnetic properties of the nanocrystals were probed by electron paramagnetic resonance EPR . Structural characterization by means of x-ray diffraction and transmission electron microscopy gave no evidence of second phase formation within the detection limits of the used equipment. The EPR analysis was carried out by simulations of the powderlike EPR spectra. The results confirm that in the core of these nanocrystals Co was incorporated as Co2+, occupying the Zn2+ sites in the wurtzite structure of ZnO. Additionally we identify two Co signals stemming from the nanocrystals’ shell. The performed surface modifications clearly change the relative intensity of the EPR spectrum components, revealing the core and shell signals

A pseudopotential study of electron-hole excitations in colloidal, free-standing InAs quantum dots

Excitonic spectra are calculated for free-standing, surface passivated InAs quantum dots using atomic pseudopotentials for the single-particle states and screened Coulomb interactions for the two-body terms. We present an analysis of the single particle states involved in each excitation in terms of their angular momenta and Bloch-wave parentage. We find that (i) in agreement with other pseudopotential studies of CdSe and InP quantum dots, but in contrast to k.p calculations, dot states wavefunction exhibit strong odd-even angular momentum envelope function mixing (e.g. $s$ with $p$) and large valence-conduction coupling. (ii) While the pseudopotential approach produced very good agreement with experiment for free-standing, colloidal CdSe and InP dots, and for self-assembled (GaAs-embedded) InAs dots, here the predicted spectrum does {\em not} agree well with the measured (ensemble average over dot sizes) spectra. (1) Our calculated excitonic gap is larger than the PL measure one, and (2) while the spacing between the lowest excitons is reproduced, the spacings between higher excitons is not fit well. Discrepancy (1) could result from surface states emission. As for (2), agreement is improved when account is taken of the finite size distribution in the experimental data. (iii) We find that the single particle gap scales as $R^{-1.01}$ (not $R^{-2}$), that the screened (unscreened) electron-hole Coulomb interaction scales as $R^{-1.79}$ ($R^{-0.7}$), and that the eccitonic gap sclaes as $R^{-0.9}$. These scaling laws are different from those expected from simple models.Comment: 12 postscript figure

Equilibrium shapes and energies of coherent strained InP islands

The equilibrium shapes and energies of coherent strained InP islands grown on GaP have been investigated with a hybrid approach that has been previously applied to InAs islands on GaAs. This combines calculations of the surface energies by density functional theory and the bulk deformation energies by continuum elasticity theory. The calculated equilibrium shapes for different chemical environments exhibit the {101}, {111}, {\=1\=1\=1} facets and a (001) top surface. They compare quite well with recent atomic-force microscopy data. Thus in the InP/GaInP-system a considerable equilibration of the individual islands with respect to their shapes can be achieved. We discuss the implications of our results for the Ostwald ripening of the coherent InP islands. In addition we compare strain fields in uncapped and capped islands.Comment: 10 pages including 6 figures. Submitted to Phys. Rev. B. Related publications can be found at http://www.fhi-berlin.mpg.de/th/paper.htm

Revealing the Two-Electron Cusp in the Ground States of He and H2 via Quasifree Double Photoionization

We report on kinematically complete measurements and ab initio non-perturbative calculations of double ionization of He and H2 by a single 800 eV circularly polarized photon. We confirm the quasifree mechanism of photoionization for H2 and show how it originates from the two-electron cusp in the ground state of a two-electron target. Our approach establishes a new method for mapping electrons relative to each other and provides valuable insight into photoionization beyond the electric-dipole approximation.Comment: 7 pages, 4 figure

Tight-binding study of the influence of the strain on the electronic properties of InAs/GaAs quantum dots

We present an atomistic investigation of the influence of strain on the electronic properties of quantum dots (QD's) within the empirical $s p^{3} s^{*}$ tight-binding (ETB) model with interactions up to 2nd nearest neighbors and spin-orbit coupling. Results for the model system of capped pyramid-shaped InAs QD's in GaAs, with supercells containing $10^{5}$ atoms are presented and compared with previous empirical pseudopotential results. The good agreement shows that ETB is a reliable alternative for an atomistic treatment. The strain is incorporated through the atomistic valence force field model. The ETB treatment allows for the effects of bond length and bond angle deviations from the ideal InAs and GaAs zincblende structure to be selectively removed from the electronic-structure calculation, giving quantitative information on the importance of strain effects on the bound state energies and on the physical origin of the spatial elongation of the wave functions. Effects of dot-dot coupling have also been examined to determine the relative weight of both strain field and wave function overlap.Comment: 22 pages, 7 figures, submitted to Phys. Rev. B (in press) In the latest version, added Figs. 3 and 4, modified Fig. 5, Tables I and II,.and added new reference

Multiband tight-binding theory of disordered ABC semiconductor quantum dots: Application to the optical properties of alloyed CdZnSe nanocrystals

Zero-dimensional nanocrystals, as obtained by chemical synthesis, offer a broad range of applications, as their spectrum and thus their excitation gap can be tailored by variation of their size. Additionally, nanocrystals of the type ABC can be realized by alloying of two pure compound semiconductor materials AC and BC, which allows for a continuous tuning of their absorption and emission spectrum with the concentration x. We use the single-particle energies and wave functions calculated from a multiband sp^3 empirical tight-binding model in combination with the configuration interaction scheme to calculate the optical properties of CdZnSe nanocrystals with a spherical shape. In contrast to common mean-field approaches like the virtual crystal approximation (VCA), we treat the disorder on a microscopic level by taking into account a finite number of realizations for each size and concentration. We then compare the results for the optical properties with recent experimental data and calculate the optical bowing coefficient for further sizes

Optical anisotropy in vertically coupled quantum dots

We have studied the polarization of surface and edge-emitted photoluminescence (PL) from structures with vertically coupled In0.5Ga0.5As/GaAs quantum dots (QD’s) grown by molecular beam epitaxy. The PL polarization is found to be strongly dependent on the number of stacked layers. While single-layer and 3-layer structures show only a weak TE polarization, it is enhanced for 10-layer stacks. The 20-layer stacks additionally show a low-energy side-band of high TE polarization, which is attributed to laterally coupled QD’s forming after the growth of many layers by lateral coalescence of QD’s in the upper layers. While in the single, 3- and 10-layer stacks, both TE polarized PL components are stronger than the TM component, the [110] TE component is weaker than the TM component in the 20-layer stack. This polarization reversal is attributed to an increasing vertical coupling with increasing layer number due to increasing dot size

Exciton dephasing and biexciton binding in CdSe/ZnSe islands

The dephasing of excitons and the formation of biexcitons in self-organized CdSe/ZnSe islands grown by molecular-beam epitaxy is investigated using spectrally resolved four-wave mixing. A distribution of exciton-exciton scattering efficiencies and dephasing times in the range of 0.5–10 ps are observed. This indicates the presence of differently localized exciton states at comparable transition energies. Polarization-dependent measurements identify the formation of biexcitons with a biexciton binding energy of more than four times the bulk value. With decreasing exciton energy, the binding energy slightly increases from 21.5 to 23 meV, while its broadening decreases from 5.5 to 3 meV. This is attributed to a strong three-dimensional confinement with improving shape uniformity for decreasing exciton energy

The Aharonov-Bohm effect for an exciton

We study theoretically the exciton absorption on a ring shreded by a magnetic flux. For the case when the attraction between electron and hole is short-ranged we get an exact solution of the problem. We demonstrate that, despite the electrical neutrality of the exciton, both the spectral position of the exciton peak in the absorption, and the corresponding oscillator strength oscillate with magnetic flux with a period $\Phi_0$---the universal flux quantum. The origin of the effect is the finite probability for electron and hole, created by a photon at the same point, to tunnel in the opposite directions and meet each other on the opposite side of the ring.Comment: 13 RevTeX 3.0 pages plus 4 EPS-figures, changes include updated references and an improved chapter on possible experimental realization

Excitons, biexcitons, and phonons in ultrathin CdSe/ZnSe quantum structures

The optical properties of CdSe nanostructures grown by migration-enhanced epitaxy of CdSe on ZnSe are studied by time-, energy-, and temperature-dependent photoluminescence and excitation spectroscopy, as well as by polarization-dependent four-wave mixing and two-photon absorption experiments. The nanostructures consist of a coherently strained Zn1−xCdxSe/ZnSe quantum well with embedded islands of higher Cd content with sizes of a few nanometer due to strain-induced CdSe accumulation. The local increase in CdSe concentration results in a strong localization of the excitonic wave function, in an increase in radiative lifetime, and a decrease of the dephasing rate. Local LO-phonon modes caused by the strong modulation of the Cd concentration profile are found in phonon-assisted relaxation processes. Confined biexcitons with large binding energies between 20 and 24 meV are observed, indicating the important role of biexcitons even at room temperature