179 research outputs found
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
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
New Mechanism for Electronic Energy Relaxation in Nanocrystals
The low-frequency vibrational spectrum of an isolated nanometer-scale solid
differs dramatically from that of a bulk crystal, causing the decay of a
localized electronic state by phonon emission to be inhibited. We show,
however, that an electron can also interact with the rigid translational motion
of a nanocrystal. The form of the coupling is dictated by the equivalence
principle and is independent of the ordinary electron-phonon interaction. We
calculate the rate of nonradiative energy relaxation provided by this mechanism
and establish its experimental observability.Comment: 4 pages, Submitted to Physical Review
Tight-Binding model for semiconductor nanostructures
An empirical tight-binding (TB) model is applied to the
investigation of electronic states in semiconductor quantum dots. A basis set
of three -orbitals at the anions and one -orbital at the cations is
chosen. Matrix elements up to the second nearest neighbors and the spin-orbit
coupling are included in our TB-model. The parametrization is chosen so that
the effective masses, the spin-orbit-splitting and the gap energy of the bulk
CdSe and ZnSe are reproduced. Within this reduced TB-basis the
valence (p-) bands are excellently reproduced and the conduction (s-) band is
well reproduced close to the -point, i.e. near to the band gap. In
terms of this model much larger systems can be described than within a (more
realistic) -basis. The quantum dot is modelled by using the (bulk)
TB-parameters for the particular material at those sites occupied by atoms of
this material. Within this TB-model we study pyramidal-shaped CdSe quantum dots
embedded in a ZnSe matrix and free spherical CdSe quantum dots (nanocrystals).
Strain-effects are included by using an appropriate model strain field. Within
the TB-model, the strain-effects can be artifically switched off to investigate
the infuence of strain on the bound electronic states and, in particular, their
spatial orientation. The theoretical results for spherical nanocrystals are
compared with data from tunneling spectroscopy and optical experiments.
Furthermore the influence of the spin-orbit coupling is investigated
Tuning trion binding energy and oscillator strength in a laterally finite 2D system: CdSe nanoplatelets as a model system for trion properties
We present a theoretical study combined with experimental validations demonstrating that CdSe nanoplatelets are a model system to investigate the tunability of trions and excitons in laterally finite 2D semiconductors. Our results show that the trion binding energy can be tuned from 36 meV to 18 meV with the lateral size and decreasing aspect ratio, while the oscillator strength ratio of trions to excitons decreases. In contrast to conventional quantum dots, the trion oscillator strength in a nanoplatelet at low temperature is smaller than that of the exciton. The trion and exciton Bohr radii become lateral size tunable, e.g. from ∼3.5 to 4.8 nm for the trion. We show that dielectric screening has strong impact on these properties. By theoretical modeling of transition energies, binding energies and oscillator strength of trions and excitons and comparison with experimental findings, we demonstrate that these properties are lateral size and aspect ratio tunable and can be engineered by dielectric confinement, allowing to suppress e.g. detrimental trion emission in devices. Our results strongly impact further in-depth studies, as the demonstrated lateral size tunable trion and exciton manifold is expected to influence properties like gain mechanisms, lasing, quantum efficiency and transport even at room temperature due to the high and tunable trion binding energies.EC/H2020/714876/EU/Photonics in Flatland: Band Structure Engineering of 2D Excitons in Fluorescent Colloidal Nanomaterials/PHOCONATU Berlin, Open-Access-Mittel - 202
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
A comparative study demonstrates strong size tunability of carrier–phonon coupling in CdSe-based 2D and 0D nanocrystals
In a comparative study we investigate the carrier–phonon coupling in CdSe based core-only and hetero 2D as well as 0D nanoparticles. We demonstrate that the coupling can be strongly tuned by the lateral size of nanoplatelets, while, due to the weak lateral confinement, the transition energies are only altered by tens of meV. Our analysis shows that an increase in the lateral platelet area results in a strong decrease in the phonon coupling to acoustic modes due to deformation potential interaction, yielding an exciton deformation potential of 3.0 eV in line with theory. In contrast, coupling to optical modes tends to increase with the platelet area. This cannot be explained by Fröhlich interaction, which is generally dominant in II–VI materials. We compare CdSe/CdS nanoplatelets with their equivalent, spherical CdSe/CdS nanoparticles. Universally, in both systems the introduction of a CdS shell is shown to result in an increase of the average phonon coupling, mainly related to an increase of the coupling to acoustic modes, while the coupling to optical modes is reduced with increasing CdS layer thickness. The demonstrated size and CdS overgrowth tunability has strong implications for applications like tuning carrier cooling and carrier multiplication – relevant for solar energy harvesting applications. Other implications range from transport in nanosystems e.g. for field effect transistors or dephasing control. Our results open up a new toolbox for the design of photonic materials.TU Berlin, Open-Access-Mittel - 201
Radiative corrections to the excitonic molecule state in GaAs microcavities
The optical properties of excitonic molecules (XXs) in GaAs-based quantum
well microcavities (MCs) are studied, both theoretically and experimentally. We
show that the radiative corrections to the XX state, the Lamb shift
and radiative width , are
large, about of the molecule binding energy , and
definitely cannot be neglected. The optics of excitonic molecules is dominated
by the in-plane resonant dissociation of the molecules into outgoing
1-mode and 0-mode cavity polaritons. The later decay channel,
``excitonic molecule 0-mode polariton + 0-mode
polariton'', deals with the short-wavelength MC polaritons invisible in
standard optical experiments, i.e., refers to ``hidden'' optics of
microcavities. By using transient four-wave mixing and pump-probe
spectroscopies, we infer that the radiative width, associated with excitonic
molecules of the binding energy meV, is
meV in the microcavities and
meV in a reference GaAs single quantum
well (QW). We show that for our high-quality quasi-two-dimensional
nanostructures the limit, relevant to the XX states, holds at
temperatures below 10 K, and that the bipolariton model of excitonic molecules
explains quantitatively and self-consistently the measured XX radiative widths.
We also find and characterize two critical points in the dependence of the
radiative corrections against the microcavity detuning, and propose to use the
critical points for high-precision measurements of the molecule bindingenergy
and microcavity Rabi splitting.Comment: 16 pages, 11 figures, accepted for publication in Phys. Rev.
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
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