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Register a new userA pseudopotential study of electron-hole excitations in colloidal, free-standing InAs quantum dots
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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.
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We use a many-body, atomistic empirical pseudopotential approach to predict the multi-exciton emission spectrum of a lens shaped InAs/GaAs self-assembled quantum dot. We discuss the effects of (i) The direct Coulomb energies, including the differences of electron and hole wavefunctions, (ii) the exchange Coulomb energies and (iii) correlation energies given by a configuration interaction calculation. Emission from the groundstate of the $N$ exciton system to the $N-1$ exciton system involving $e_0to h_0$ and $e_1to h_1$ recombinations are discussed. A comparison with a simpler single-band, effective mass approach is presented.
We present a comprehensive study of the optical properties of InAs/InP self-assembled quantum dots (QDs) using an empirical pseudopotential method and configuration interaction treatment of the many-particle effects. The results are compared to those of InAs/GaAs QDs. The main results are: (i) The alignment of emission lines of neutral exciton, charged exciton and biexciton in InAs/InP QDs is quite different from that in InAs/GaAs QDs. (ii) The hidden correlation in InAs/InP QDs is 0.7 - 0.9 meV, smaller than that in InAs/GaAs QDs. (iii) The radiative lifetimes of neutral exciton, charged exciton and biexciton in InAs/InP QDs are about twice longer than those in InAs/GaAs QDs. (v) The phase diagrams of few electrons and holes in InAs/InP QDs differ greatly from those in InAs/GaAs QDs. The filling orders of electrons and holes are shown to obey the Hunds rule and Aufbau principle, and therefore the photoluminescence spectra of highly charged excitons are very different from those of InAs/GaAs QDs.
Free-standing nanoribbons of InAs quantum membranes (QMs) transferred onto a (Si/Mo) multilayer mirror substrate are characterized by hard x-ray photoemission spectroscopy (HXPS), and by standing-wave HXPS (SW-HXPS). Information on the chemical composition and on the chemical states of the elements within the nanoribbons was obtained by HXPS and on the quantitative depth profiles by SW-HXPS. By comparing the experimental SW-HXPS rocking curves to x-ray optical calculations, the chemical depth profile of the InAs(QM) and its interfaces were quantitatively derived with angstrom precision. We determined that: i) the exposure to air induced the formation of an InAsO$_4$ layer on top of the stoichiometric InAs(QM); ii) the top interface between the air-side InAsO$_4$ and the InAs(QM) is not sharp, indicating that interdiffusion occurs between these two layers; iii) the bottom interface between the InAs(QM) and the native oxide SiO$_2$ on top of the (Si/Mo) substrate is abrupt. In addition, the valence band offset (VBO) between the InAs(QM) and the SiO$_2$/(Si/Mo) substrate was determined by HXPS. The value of $VBO = 0.2 pm 0.04$ eV is in good agreement with literature results obtained by electrical characterization, giving a clear indication of the formation of a well-defined and abrupt InAs/SiO$_2$ heterojunction. We have demonstrated that HXPS and SW-HXPS are non-destructive, powerful methods for characterizing interfaces and for providing chemical depth profiles of nanostructures, quantum membranes, and 2D layered materials.
We investigate the addition spectrum of a graphene quantum dot in the vicinity of the electron-hole crossover as a function of perpendicular magnetic field. Coulomb blockade resonances of the 50 nm wide dot are visible at all gate voltages across the transport gap ranging from hole to electron transport. The magnetic field dependence of more than 50 states displays the unique complex evolution of the diamagnetic spectrum of a graphene dot from the low-field regime to the Landau regime with the n=0 Landau level situated in the center of the transport gap marking the electron-hole crossover. The average peak spacing in the energy region around the crossover decreases with increasing magnetic field. In the vicinity of the charge neutrality point we observe a well resolved and rich excited state spectrum.
We present experimental magnetotunneling results and atomistic pseudopotential calculations of quasiparticle electron and hole wave functions of self-assembled InAs/GaAs quantum dots. The combination of a predictive theory along with the experimental results allows us to gain direct insight into the quantum states. We monitor the effects of (i) correlations, (ii) atomistic symmetry and (iii) piezoelectricity on the confined carriers and (iv) observe a peculiar charging sequence of holes that violates the Aufbau principle.
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