The effect of small elongations on the electronic and optical signatures in InAs nanocrystal quantum dots

We present a detailed theoretical investigation of the electronic structure and optical properties of InAs nanocrystals at the transition from spheres to rods. Using a semiempirical pseudopotential approach, we predict that, despite the qualitative similarity of both intra- and inter-band optical spectra, for NCs with R > 15 °A even slight elongations should result in shifts of the order of hundreds of meV in the spacings between STM peaks measured in the positive bias regime, in the position of the intra- band absorption peaks associated with transitions in the conduction band and in the separation between the first and the fifth peak in PLE experiments. Our results show that, based on the spectroscopic data, it should be possible to discriminate between spherical and elongated NCs with aspect ratios of length over diameter as small as 1.2. Indeed our results suggest that many nominally spherical experimental samples contained a large fraction of slightly elongated structures

Collective effects in charge transfer within a hybrid organic-inorganic system

A collective electron transfer (ET) process was discovered by studying the current noise in a field effect transistor with light-sensitive gate formed by nanocrystals linked by organic molecules to its surface. Fluctuations in the ET through the organic linker are reflected in the fluctuations of the transistor conductivity. The current noise has an avalanche character. Critical exponents obtained from the noise power spectra, avalanche distributions, and the dependence of the average avalanche size on avalanche duration are consistent with each other. A plausible model is proposed for this phenomenonComment: 15 pages 4 figures. Accepted for publication in Physical Review Letter

Size dependent tunneling and optical spectroscopy of CdSe quantum rods

Photoluminescence excitation spectroscopy and scanning tunneling spectroscopy are used to study the electronic states in CdSe quantum rods that manifest a transition from a zero dimensional to a one dimensional quantum confined structure. Both optical and tunneling spectra show that the level structure depends primarily on the rod diameter and not on length. With increasing diameter, the band-gap and the excited state level spacings shift to the red. The level structure was assigned using a multi-band effective-mass model, showing a similar dependence on rod dimensions.Comment: Accepted to PRL (nearly final version). 4 pages in revtex, 4 figure

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

Higher-Derivative Terms in N=2 Supersymmetric Effective Actions

We show how to systematically construct higher-derivative terms in effective actions in harmonic superspace despite the infinite redundancy in their description due to the infinite number of auxiliary fields. Making an assumption about the absence of certain superspace Chern-Simons-like terms involving vector multiplets, we write all 3- and 4-derivative terms on Higgs, Coulomb, and mixed branches. Among these terms are several with only holomorphic dependence on fields, and at least one satisfies a non-renormalization theorem. These holomorphic terms include a novel 3-derivative term on mixed branches given as an integral over 3/4 of superspace. As an illustration of our method, we search for Wess-Zumino terms in the low energy effective action of N=2 supersymmetric QCD. We show that such terms occur only on mixed branches. We also present an argument showing that the combination of space-time locality with supersymmetry implies locality in the anticommuting superspace coordinates of for unconstrained superfields.Comment: 30 pages. Added references and simplified final form of WZ ter

Driving current through single organic molecules

We investigate electronic transport through two types of conjugated molecules. Mechanically controlled break-junctions are used to couple thiol endgroups of single molecules to two gold electrodes. Current-voltage characteristics (IVs) of the metal-molecule-metal system are observed. These IVs reproduce the spatial symmetry of the molecules with respect to the direction of current flow. We hereby unambigously detect an intrinsic property of the molecule, and are able to distinguish the influence of both the molecule and the contact to the metal electrodes on the transport properties of the compound system.Comment: 4 pages, 5 figure

Electrical transport through single-molecule junctions: from molecular orbitals to conduction channels

We present an atomistic theory of electronic transport through single organic molecules that reproduces the important features of the current-voltage characteristics observed in recent experiments. We trace these features to their origin in the electronic structure of the molecules and their local atomic environment. We demonstrate how conduction channels arise from the molecular orbitals and elucidate which specific properties of the individual orbitals determine their contribution to the current.Comment: Revtex4, 4 pages, 4 figures. Version with color figures in http://www-tfp.physik.uni-karlsruhe.de/~cuevas/Publications.htm

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]

Imaging and spectroscopy of artificial-atom states in core/shell nanocrystal quantum dots

Current imaging scanning tunneling microscopy is used to observe the electronic wavefunctions in InAs/ZnSe core/shell nanocrystals. Images taken at a bias corresponding to the s conduction band state show that it is localized in the central core region, while images at higher bias probing the p state reveal that it extends to the shell. This is supported by optical and tunneling spectroscopy data demonstrating that the s-p gap closes upon shell growth. Shapes of the current images resemble atom-like envelope wavefunctions of the quantum dot calculated within a particle in a box model.Comment: to be published in Physical Review Letter