Oxidative cleavage of carotenoids catalyzed by enzyme models and beta-carotene 15,15´-monooxygenase

The enzyme that catalyzes the central cleavage of β-carotene is an iron monooxygenase. The protein was isolated from chicken intestinal mucosa and overexpressed in two different cell lines. Inductively coupled plasma (ICP) emission analysis revealed that the hydrophobic 60.3-kDa enzyme contains one iron/mole protein. The substrate specificity was investigated, and the reaction mechanism elucidated incubating α-carotene in the presence of highly enriched 17O2 and H218O. A supramolecular enzyme model was synthesized, binding carotenoids Ka > 106 mol-1, which mimics the regiospecific enzymatic cleavage of carotenoid

Reducing decoherence of the confined exciton state in a quantum dot by pulse-sequence control

We study the phonon-induced dephasing of the exciton state in a quantum dot excited by a sequence of ultra-short pulses. We show that the multiple-pulse control leads to a considerable improvement of the coherence of the optically excited state. For a fixed control time window, the optimized pulsed control often leads to a higher degree of coherence than the control by a smooth single Gaussian pulse. The reduction of dephasing is considerable already for 2-3 pulses.Comment: Final version (moderate changes

Experimental imaging and atomistic modeling of electron and hole quasiparticle wave functions in InAs/GaAs quantum dots

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.Comment: Submitted to Physical Review B. A version of this paper with figures can be found at http://www.sst.nrel.gov/nano_pub/mts_preprint.pd

A Large Blue Shift of the Biexciton State in Tellurium Doped CdSe Colloidal Quantum Dots

The exciton-exciton interaction energy of Tellurium doped CdSe colloidal quantum dots is experimentally investigated. The dots exhibit a strong Coulomb repulsion between the two excitons, which results in a huge measured biexciton blue shift of up to 300 meV. Such a strong Coulomb repulsion implies a very narrow hole wave function localized around the defect, which is manifested by a large Stokes shift. Moreover, we show that the biexciton blue shift increases linearly with the Stokes shift. This result is highly relevant for the use of colloidal QDs as optical gain media, where a large biexciton blue shift is required to obtain gain in the single exciton regime.Comment: 9 pages, 4 figure

Full configuration interaction approach to the few-electron problem in artificial atoms

We present a new high-performance configuration interaction code optimally designed for the calculation of the lowest energy eigenstates of a few electrons in semiconductor quantum dots (also called artificial atoms) in the strong interaction regime. The implementation relies on a single-particle representation, but it is independent of the choice of the single-particle basis and, therefore, of the details of the device and configuration of external fields. Assuming no truncation of the Fock space of Slater determinants generated from the chosen single-particle basis, the code may tackle regimes where Coulomb interaction very effectively mixes many determinants. Typical strongly correlated systems lead to very large diagonalization problems; in our implementation, the secular equation is reduced to its minimal rank by exploiting the symmetry of the effective-mass interacting Hamiltonian, including square total spin. The resulting Hamiltonian is diagonalized via parallel implementation of the Lanczos algorithm. The code gives access to both wave functions and energies of first excited states. Excellent code scalability in a parallel environment is demonstrated; accuracy is tested for the case of up to eight electrons confined in a two-dimensional harmonic trap as the density is progressively diluted and correlation becomes dominant. Comparison with previous Quantum Monte Carlo simulations in the Wigner regime demonstrates power and flexibility of the method.Comment: RevTeX 4.0, 18 pages, 6 tables, 9 postscript b/w figures. Final version with new material. Section 6 on the excitation spectrum has been added. Some material has been moved to two appendices, which appear in the EPAPS web depository in the published versio

From Bioorganic Chemistry to Catalysis

Research projects of the Department of Chemistry, University of Basel are reviewed ranging from the synthesis of complex natural products to the development of metalorganic catalysts and organocatalyst

Electron microscopic and optical investigations of the indium distribution GaAs capped InxGa1-xAs islands

Results from a structural and optical analysis of buried InxGa1-xAs islands carried out after the process of GaAs overgrowth are presented. It is found that during the growth process, the indium concentration profile changes and the thickness of the wetting layer emanating from a Stranski-Krastanow growth mode grows significantly. Quantum dots are formed due to strong gradients in the indium concentration, which is demonstrated by photoluminescence and excitation spectroscopy of the buried InxGa1-xAs islands. (C) 1997 American Institute of Physics

Stability of quantum-dot excited-state laser emission under simultaneous ground-state perturbation

The impact of ground state amplification on the laser emission of In(Ga)As quantum dot excited state lasers is studied in time-resolved experiments. We find that a depopulation of the quantum dot ground state is followed by a drop in excited state lasing intensity. The magnitude of the drop is strongly dependent on the wavelength of the depletion pulse and the applied injection current. Numerical simulations based on laser rate equations reproduce the experimental results and explain the wavelength dependence by the different dynamics in lasing and non-lasing sub-ensembles within the inhomogeneously broadened quantum dots. At high injection levels, the observed response even upon perturbation of the lasing sub-ensemble is small and followed by a fast recovery, thus supporting the capacity of fast modulation in dual-state devices