Colloidal synthesis and optical properties of type-II CdSe-CdTe and inverted CdTe-CdSe core-wing heteronanoplatelets.

We developed colloidal synthesis to investigate the structural and electronic properties of CdSe-CdTe and inverted CdTe-CdSe heteronanoplatelets and experimentally demonstrate that the overgrowth of cadmium selenide or cadmium telluride core nanoplatelets with counterpartner chalcogenide wings leads to type-II heteronanoplatelets with emission energies defined by the bandgaps of the CdSe and CdTe platelets and the characteristic band offsets. The observed conduction and valence band offsets of 0.36 eV and 0.56 eV are in line with theoretical predictions. The presented type-II heteronanoplatelets exhibit efficient spatially indirect radiative exciton recombination with a quantum yield as high as 23%. While the exciton lifetime is strongly prolonged in the investigated type-II 2D systems with respect to 2D type-I systems, the occurring 2D giant oscillator strength (GOST) effect still leads to a fast and efficient exciton recombination. This makes type-II heteronanoplatelets interesting candidates for low threshold lasing applications and photovoltaics.

Pump-probe quantum state tomography in a semiconductor optical amplifier.

Pump-probe quantum state tomography was applied to the transmission of a coherent state through an In(Ga)As based quantum dot optical amplifier during the interaction with an optical pump pulse. The Wigner function and the statistical moments of the field were extracted and used to determine the degree of population inversion and the signal-to-noise ratio in a sub-picosecond time window.

Improving carrier injection in colloidal CdSe nanocrystals by embedding them in a pseudomorphic ZnSe/ZnMgSe quantum well structure.

The incorporation of colloidal nanocrystals in a high crystalline quality semiconductor matrix, the efficient carrier injection into the embedded nanocrystals and the fast optical response are key features for the fabrication of novel optoelectronic nanodevices based on colloidal nanostructures as active optical material. Using a novel growth approach, colloidal bare CdSe and core-shell CdSe/ZnS nanocrystals were monolithically incorporated in pseudomorphic ZnSe/ZnMgSe quantum wells in order to control and enhance the carrier transfer into the nanocrystals. The photoluminescence for bare CdSe nanocrystals incorporated in ZnSe/ZnMgSe quantum well structures is substantially enhanced in comparison to nanocrystals sandwiched in ZnSe epilayers, which we attribute to increased carrier injection into the embedded nanocrystals via the quantum well, resembling the function of a wetting layer in Stranski-Krastanov-grown quantum dots. Core-shell CdSe/ZnS nanocrystals embedded in quantum well structures do not show considerable PL modifications because the ZnS shell prevents the efficient carrier migration between the nanocrystal and the matrix. Systematic investigations of structural and optical properties by high-resolution x-ray diffraction, temperature-dependent photoluminescence and time-resolved emission are presented.

Impact of Coulomb scattering on the ultrafast gain recovery in InGaAs quantum dots.

The application of quantum dot (QD) semiconductor optical amplifiers (SOAs) in above 100-Gbit Ethernet networks demands an ultrafast gain recovery on time scales similar to that of the input pulse approximately 100 GHz repetition frequency. Microscopic scattering processes have to act at shortest possible time scales and mechanisms speeding up the Coulomb scattering have to be explored, controlled, and exploited. We present a microscopic description of the gain recovery by coupled polarization- and population dynamics in a thermal nonequilibrium situation going beyond rate-equation models and discuss the limitations of Coulomb scattering between 0D and 2D-confined quantum states. An experiment is designed which demonstrates the control of gain recovery for THz pulse trains in InGaAs QD-based SOAs under powerful electrical injection.

Exciton-plasmon-photon conversion in plasmonic nanostructures.

A silver-nanowire cavity is functionalized with CdSe nanocrystals and optimized towards cavity quantum electrodynamics by varying the nanocrystal-nanowire distance d and cavity length L. From the modulation of the nanocrystal emission by the cavity modes a plasmon group velocity of v (gr) approximately 0.5c is derived. Efficient exciton-plasmon-photon conversion and guiding is demonstrated along with a modification in the spontaneous emission rate of the coupled exciton-plasmon system.

Cavity QED with semiconductor nanocrystals.

We report on a strongly coupled cavity quantum electrodynamic (CQED) system consisting of a CdSe nanocrystal coupled to a single photon mode of a polymer microsphere. The strong exciton-photon coupling is manifested by the observation of a cavity mode splitting variant Planck's over 2piOmega(exp) between 30 und 45 microeV and photon lifetime measurements of the coupled exciton-photon state. The single photon mode is isolated by lifting the mode degeneracy in a slightly deformed microsphere cavity and addressing it by high-resolution imaging spectroscopy. This cavity mode is coupled to a localized exciton of an anisotropically shaped CdSe nanocrystal that emits highly polarized light in resonance to the cavity mode and that was placed in the maximum electromagnetic field close to the microsphere surface. The exciton confined in the CdSe nanorod exhibits an optical transition dipole moment much larger than that of atoms, the standard system for CQED experiments, and a low-temperature homogeneous line width much narrower than the high-Q cavity mode width. The observation of strong coupling in a colloidal semiconductor nanocrystal-cavity system opens the way to study fundamental quantum-optics phenomena and to implement quantum information processing concepts that work in the visible spectral range and are based on solid-state nanomaterials.

Recombination dynamics of CdTe/CdS core-shell nanocrystals.

The recombination dynamics of zinc-blende-type, deep-red emitting CdTe/CdS core-shell nanocrystals is studied over a wide temperature range. Two characteristic decay regimes are found: a temperature-dependent decay component of a few nanoseconds and a long-living temperature-independent component of approximately 315 ns. The average decay time of the exciton states changes from 20 to 5ns when the temperature is increased from 15 to 295 K. At low temperatures, the observed decay behavior is assigned to thermally induced population and decay of the allowed exchange-split exciton states. At temperatures above T>100 K, nonradiative decay channels involving phonons start to contribute to the exciton recombination. The observed broad distribution in decay times, monitored by stretched exponential fitting functions, we explain by variations in the electron-hole overlap caused by a partly incomplete CdTe/CdS core-shell structure and the nearly energy-degenerated bright and dark state superposition.

Hybrid epitaxial-colloidal semiconductor nanostructures.

We present a growth technique which combines wet-chemical growth and molecular beam epitaxy (MBE) to create complex semiconductor nanostructures with nanocrystals as active optical material. The obtained results show that wet-chemically prepared semiconductor nanocrystals can be incorporated in an epitaxally grown crystalline cap layer. As an exemplary system we chose CdSe nanorods and CdSe(ZnS) core-shell nanocrystals in ZnSe and discuss the two limits of thin (d approximately 2R) and thick (d>2R) ZnSe cap layers of thickness d for CdSe nanorods and nanodots of radii R between 2 and 4 nm. In contrast to the strain-induced CdSe/ZnSe Stranski-Krastanow growth of a quantum dot layer in a semiconductor heterostructure, the technique proposed here does not rely on strain and thus results in additional degrees of freedom for choosing composition, concentration, shape, and size of the nanocrystals. Transmission electron microscopy and X-ray diffractometry show that the ZnSe cap layer is of high crystalline quality and provides all parameters for a consecutive growth of Bragg structures, waveguides, or diode structures for electrical injection.

Exciton fine structure in single CdSe nanorods.

We study the optical properties of excitons in one-dimensional (1D) nanostructures at low temperatures. In single CdSe/ZnS core-shell nanorods we observe a fine structure splitting and explain it by exchange interaction. Two peaks are observed with different degrees of linear polarization of DLP<0.85 and DLP>0.95. For small nanorod radii R< or =a(B)/2, an increase in the photoluminescence decay time is found when the temperature increases from 10 to 80 K. The observations are explained by a radius-dependent change in the symmetry of the 1D-exciton ground state which transforms from a dark state into bright states below a critical radius of R(crit) approximately 3.7 nm.

Coherent control and polarization readout of individual excitonic states.

We present measurements and simulations of coherent control and readout of the polarization in individual exciton states. The readout is accomplished by transient four-wave mixing detected by heterodyne spectral interferometry. We observe Rabi oscillations in the polarization, which show half the period of the Rabi oscillations in the population. A decrease of the oscillation amplitude with pulse area is observed, which is not accompanied by a change in the dephasing time. This suggests the transfer of the excitation to other states as the origin of the Rabi-oscillation damping. Detuning of the excitation enables the control of the polarization in phase and amplitude and is in qualitative agreement with simulations for a two-level system. Additionally, simultaneous Rabi flopping of several spatially and energetically close exciton states is demonstrated.

Exciton dephasing in quantum dot molecules.

We have measured the exciton dephasing time in InAs/GaAs quantum dot molecules having different interdot barrier thicknesses in the temperature range from 5 to 60 K, using a highly sensitive four-wave mixing heterodyne technique. At 5 K dephasing times of several hundred picoseconds are found. Moreover, a systematic dependence of the dephasing dynamics on the barrier thickness is observed. These results show how the quantum-mechanical coupling of the electronic wave functions in the molecules affects both the exciton radiative lifetime and the exciton-acoustic phonon interaction.

Relaxation and dephasing of multiexcitons in semiconductor quantum dots.

We measure the dephasing time of ground-state excitonic transitions in InGaAs quantum dots under electrical injection in the temperature range from 10 to 70 K. Electrical injection into the barrier region results in a pure dephasing of the excitonic transitions. Once the injected carriers fill the electronic ground state, the biexciton to exciton transition is probed and a correlation of the exciton and biexciton phonon scattering mechanisms is found. Additional filling of the excited states creates multiexcitons that show a fast dephasing due to population relaxation.

Ultralong dephasing time in InGaAs quantum dots.

We measure a dephasing time of several hundred picoseconds at low temperature in the ground-state transition of strongly confined InGaAs quantum dots, using a highly sensitive four-wave mixing technique. Between 7 and 100 K the polarization decay has two distinct components resulting in a non-Lorentzian line shape with a lifetime-limited zero-phonon line and a broadband from elastic exciton-acoustic phonon interactions.

Biexcitonic fingerprint in the nondegenerate four-wave-mixing signal of weakly confined cadmium sulfur quantum dots.

Nondegenerate four-wave mixing is analyzed with respect to biexcitonic contributions in the third-order nonlinear susceptibility x((3)) . The presence of biexcitons causes a distinct asymmetry in the frequency dependence of self-diffraction. By measurement of the dependence of the intensity of the self-diffracted signal on detuning between the two incident laser beams, the biexciton binding energy is determined to be E(XX)=7.8 meV for cadmium sulfur quantum dots of R=7.5 nm embedded in glass. Thus, even for weakly confined II-VI quantum dots with R~2.7a(B) , a confinement-induced enhancement of E(XX) was found.

Femtosecond optical gain in strongly confined quantum dots.

Optical gain was found in strongly confined CdSe quantum dots. As a result of a multitude of one- and two-electron-hole pair transitions, the gain region is broad and quasi-continuous and stretches below the absorption edge. We present a model for gain in a quasi-zero-dimensional quantum confined semiconductor system that agrees well with the femtosecond experiments.