Lowering of surface melting temperature in atomic clusters with a nearly closed shell structure

We investigate the interplay of particle number, N, and structural properties of selected clusters with N=12 up to N=562 by employing Gupta potentials parameterized for Aluminum and extensive Monte-Carlo simulations. Our analysis focuses on closed shell structures with extra atoms. The latter can put the cluster under a significant stress and we argue that typically such a strained system exhibits a reduced energy barrier for (surface) diffusion of cluster atoms. Consequently, also its surface melting temperature, T_S, is reduced, so that T_S separates from and actually falls well below the bulk value. The proposed mechanism may be responsible for the suppression of the surface melting temperature observed in a recent experiments.Comment: 9 pages, 7 figures, 1 table, REVTeX 4; submitted to Phys.Rev.

Faraday Rotation Spectroscopy of Quantum-Dot Quantum Wells

Time-resolved Faraday rotation studies of CdS/CdSe/CdS quantum-dot quantum wells have recently shown that the Faraday rotation angle exhibits several well-defined resonances as a function of probe energy close to the absorption edge. Here, we calculate the Faraday rotation angle from the eigenstates of the quantum-dot quantum well obtained with k.p theory. We show that the large number of narrow resonances with comparable spectral weight observed in experiment is not reproduced by the level scheme of a quantum-dot quantum well with perfect spherical symmetry. A simple model for broken spherical symmetry yields results in better qualitative agreement with experiment.Comment: 9 pages, 4 figure

Spin dynamics and level structure of quantum-dot quantum wells

We have characterized CdS/CdSe/CdS quantum-dot quantum wells using time-resolved Faraday rotation (TRFR). The spin dynamics show that the electron g-factor varies as a function of quantum well width and the transverse spin lifetime of several nano-seconds is robust up to room temperature. As a function of probe energy, the amplitude of the TRFR signal shows pronounced resonances, which allow one to identify individual exciton transitions. While the TRFR data are inconsistent with the conduction and valence band level scheme of spherical quantum-dot quantum wells, a model in which broken spherical symmetry is taken into account captures the essential features.Comment: 5 pages, 3 figure

Predicion of charge separation in GaAs/AlAs cylindrical Russian Doll nanostructures

We have contrasted the quantum confinement of (i) multiple quantum wells of flat GaAs and AlAs layers, i.e. (\GaAs)_{m}/(\AlAs)_n/(\GaAs)_p/(\AlAs)_q, with (ii) ``cylindrical Russian Dolls'' -- an equivalent sequence of wells and barriers arranged as concentric wires. Using a pseudopotential plane-wave calculation, we identified theoretically a set of numbers ($m,n,p$ and $q$) such that charge separation can exist in ``cylindrical Russian Dolls'': the CBM is localized in the inner GaAs layer, while the VBM is localized in the outer GaAs layer.Comment: latex, 8 page

Multiband theory of quantum-dot quantum wells: Dark excitons, bright excitons, and charge separation in heteronanostructures

Electron, hole, and exciton states of multishell CdS/HgS/CdS quantum-dot quantum well nanocrystals are determined by use of a multiband theory that includes valence-band mixing, modeled with a 6-band Luttinger-Kohn Hamiltonian, and nonparabolicity of the conduction band. The multiband theory correctly describes the recently observed dark-exciton ground state and the lowest, optically active, bright-exciton states. Charge separation in pair states is identified. Previous single-band theories could not describe these states or account for charge separation.Comment: 10 pages of ReVTex, 6 ps figures, submitted to Phys. Rev.

Electron and hole states in quantum-dot quantum wells within a spherical 8-band model

In order to study heterostructures composed both of materials with strongly different parameters and of materials with narrow band gaps, we have developed an approach, which combines the spherical 8-band effective-mass Hamiltonian and the Burt's envelope function representation. Using this method, electron and hole states are calculated in CdS/HgS/CdS/H_2O and CdTe/HgTe/CdTe/H_2O quantum-dot quantum-well heterostructures. Radial components of the wave functions of the lowest S and P electron and hole states in typical quantum-dot quantum wells (QDQWs) are presented as a function of radius. The 6-band-hole components of the radial wave functions of an electron in the 8-band model have amplitudes comparable with the amplitude of the corresponding 2-band-electron component. This is a consequence of the coupling between the conduction and valence bands, which gives a strong nonparabolicity of the conduction band. At the same time, the 2-band-electron component of the radial wave functions of a hole in the 8-band model is small compared with the amplitudes of the corresponding 6-band-hole components. It is shown that in the CdS/HgS/CdS/H_2O QDQW holes in the lowest states are strongly localized in the well region (HgS). On the contrary, electrons in this QDQW and both electron and holes in the CdTe/HgTe/CdTe/H_2O QDQW are distributed through the entire dot. The importance of the developed theory for QDQWs is proven by the fact that in contrast to our rigorous 8-band model, there appear spurious states within the commonly used symmetrized 8-band model.Comment: 15 pages, 5 figures, E-mail addresses: [email protected], [email protected]

Electron-Hole Correlations and Optical Excitonic Gaps in Quantum-Dot Quantum Wells: Tight-Binding Approach

Electron-hole correlation in quantum-dot quantum wells (QDQW's) is investigated by incorporating Coulomb and exchange interactions into an empirical tight-binding model. Sufficient electron and hole single-particle states close to the band edge are included in the configuration to achieve convergence of the first spin-singlet and triplet excitonic energies within a few meV. Coulomb shifts of about 100 meV and exchange splittings of about 1 meV are found for CdS/HgS/CdS QDQW's (4.7 nm CdS core diameter, 0.3 nm HgS well width and 0.3 nm to 1.5 nm CdS clad thickness) which have been characterized experimentally by Weller and co-workers [ D. Schooss, A. Mews, A. Eychmuller, H. Weller, Phys. Rev. B, 49, 17072 (1994)]. The optical excitonic gaps calculated for those QDQW's are in good agreement with the experiment.Comment: 3 figures, to appear in Phys.Rev.

Effect of the Surface on the Electron Quantum Size Levels and Electron g-Factor in Spherical Semiconductor Nanocrystals

The structure of the electron quantum size levels in spherical nanocrystals is studied in the framework of an eight--band effective mass model at zero and weak magnetic fields. The effect of the nanocrystal surface is modeled through the boundary condition imposed on the envelope wave function at the surface. We show that the spin--orbit splitting of the valence band leads to the surface--induced spin--orbit splitting of the excited conduction band states and to the additional surface--induced magnetic moment for electrons in bare nanocrystals. This additional magnetic moment manifests itself in a nonzero surface contribution to the linear Zeeman splitting of all quantum size energy levels including the ground 1S electron state. The fitting of the size dependence of the ground state electron g factor in CdSe nanocrystals has allowed us to determine the appropriate surface parameter of the boundary conditions. The structure of the excited electron states is considered in the limits of weak and strong magnetic fields.Comment: 11 pages, 4 figures, submitted to Phys. Rev.

Electronic structure and optical properties of ZnS/CdS nanoheterostructures

The electronic and optical properties of spherical nanoheterostructures are studied within the semi-empirical $sp^{3}s^{*}$ tight-binding model including the spin-orbit interaction. We use a symmetry-based approach previously applied to CdSe and CdTe quantum dots. The complete one-particle spectrum is obtained by using group-theoretical methods. The excitonic eigenstates are then deduced in the configuration-interaction approach by fully taking into account the Coulomb direct and exchange interactions. Here we focus on ZnS/CdS, ZnS/CdS/ZnS and CdS/ZnS nanocrystals with particular emphasis on recently reported experimental data. The degree of carrier localization in the CdS well layer is analyzed as a function of its thickness. We compute the excitonic fine structure, i.e., the relative intensities of low-energy optical transitions. The calculated values of the absorption gap show a good agreement with the experimental ones. Enhanced resonant photoluminescence Stokes shifts are predicted.Comment: 6 pages, 4 Figures, revtex