Ensemble Of Quantum Dots Research Articles

Model for the light-induced magnetization in singly charged quantum dots

Magnetization is induced in an ensemble of quantum dots, each charged with a single electron, when it is illuminated with a short circularly polarized light pulse that is resonant with the fundamental energy gap of the quantum dots. In this investigation, a quantum-mechanical model for the light-induced magnetization is presented. The phase of the magnetization precession as a function of the strength of the magnetic field in a Voigt geometry is in excellent agreement with experimental data measured on (In,Ga)As singly charged quantum dot ensembles. It is demonstrated that the precession of the hole in the trion plays a vital role because it determines the amplitude and phase of the magnetization precession. The model could also be easily extended to describe positively charged quantum dots. We also suggest that our theory, combined with measurements of the phase as a function of magnetic field, can be used as a technique to measure the resonant trion lifetime as a function of QD emission energy.

Auger recombination in In(Ga)Sb/InAs quantum dots

We report on the epitaxial formation of type II In0.5Ga0.5Sb/InAs and InSb/InAs quantum dot ensembles using metal organic vapor phase epitaxy. Employing scanning tunneling spectroscopy, we determine spatial quantum dot dimensions smaller than the de Broglie wavelength of InGaSb, which strongly indicates a three dimensional hole confinement. Photoluminescence spectroscopy at low temperatures yields an enhanced radiative recombination in the mid-infrared regime at energies of 170–200 meV. This luminescence displays a strong excitation power dependence with a blueshift indicating a filling of excited quantum dot hole states. Furthermore, a rate equation model is used to extract the Auger recombination coefficient from the power dependent intensity at 77 K yielding values of 1.35 × 10−28 cm6/s for In0.5Ga0.5Sb/InAs quantum dots and 1.47 × 10−27 cm6/s for InSb/InAs quantum dots, which is about one order of magnitude lower as previously obtained values for InGaSb superlattices.

Efficient control of coulomb enhanced second harmonic generation from excitonic transitions in quantum dot ensembles.

In this work, the second harmonic generation from excitonic transitions in semiconductor quantum dots is computationally studied. By integrating a density matrix treatment with a partial configuration interaction approach, we obtain the second order susceptibility as a function of externally applied electric and magnetic fields for highly confined neutral and charged excitons. Our results show an enhancement in the nonlinear response with respect to analogous optical processes based on intraband transitions, and predict their efficient tunability by taking advantage of the interplay between Coulomb effects and field-driven wave function manipulation.

Dissipative Laser Bullets in a Dielectric Metamaterial with Quantum Dots

We consider the problem of formation of three-dimensional spatio-temporal dissipative solitons (laser bullets) in a dense ensemble of two-level quantum dots. The principal possibility of laser bullets generation due to the strong influence of local-field effects on propagation of optical pulses in all-dielectric metamaterials with quantum dots is predicted.

Three-Dimensional Dissipative Optical Solitons in a Dielectric Medium with Quantum Dots

We consider the problem of formation of three-dimensional spatio-temporal dissipative solitons (laser bullets) in a dense ensemble of two-level quantum dots. The principal possibility of effective laser bullets generation in an all-dielectric metamaterials with quantum dots is shown. The phenomenon arises due to the simultaneous appearance of strong local field effects and significant corrections to diffraction effects during the propagation of short optical pulses in such medium.

Cooperative Effects in Quartz Media with Quantum Dots

We theoretically consider a problem of generation of infrared pulses of superradiation (SR) in a dielectric medium hosting a dense ensemble of quantum dots produced using the narrow gap semiconductors. We have studied the influence of complex local-field corrections on cooperative optical processes in such a material due to essential modifications of the effective values of the spontaneous relaxation rates.

Superstructures from lead sulfide quantum dots

ABSTRACTThe superstructures of different morphology (superlattices and supercrystals) are obtained by self-organization of lead sulfide quantum dots (QDs) on a substrate. In contrast to the SAXS patterns of isolated QDs in solutions, the X-ray intensity from ordered superstructures is modulated by the interference from the QDs in SLs or SCs leading to occurrence of the intense peaks at small scattering angles. By indexing the peaks in the SAXS patterns it is concluded that QD SLs are close-packed QD ensembles with the lattice parameter close to the dot diameter and QD SCs have primitive orthorhombic crystal lattice. Absorption and photoluminescence bands of superstructures are also analyzed.

Photoluminescence of charged CdSe/ZnS quantum dots in the gas phase: effects of charge and heating on absorption and emission probabilities.

Gas phase spectral measurements for CdSe/ZnS core/shell nanocrystal quantum dots (QDs) before and after heating with both infrared (CO2) and visible lasers are reported. As-trapped QDs are spectrally similar to the same QDs in solution; however their photoluminescence (PL) intensities are very low, at least partly due to low absorption cross sections. After heating, the PL intensities brighten by factors ranging from ∼4 to 1800 depending on the QD size and pump laser wavelength. The emission spectra no longer resemble solution spectra and are similar, regardless of the QD diameter. Emission extends from the pump laser wavelength into the near-IR, with strong emission features above the band gap energy, between 645 and 775 nm, and in the near-infrared. Emission spectra from brightened QD ensembles, single QD aggregates, and single QD monomers are similar, showing that even single QDs support PL from a wide variety of states. The heating and cooling processes for QDs in this environment are analyzed, providing limits on the magnitudes of the absorption cross sections before and after thermal brightening. A model, based on absorption bleaching by extra electrons in the conduction band, appears to account for the changes in absorption and emission behavior induced by charging and heating.

Spin-flip Raman scattering of the resident electron in singly charged (In,Ga)As/GaAs quantum dot ensembles

Highly efficient spin-flip Raman scattering of the resident electron spin is found in singly charged (In,Ga)As/GaAs quantum dots. The applied magnetic field induces a symmetry reduction for the negatively charged exciton, which serves as intermediate scattering state, thus making the spin-flip Raman scattering of the resident electron allowed. Electron-electron exchange interaction mediates the electron spin-flip. Above a threshold magnetic field that depends on the dot size and experiment geometry, the efficiency of the scattering cross section is spectrally shifted with increasing field. This shift, which follows the electron cyclotron energy, is assigned to a hybridization of s-shell singlet and p-shell triplet states of the negatively charged exciton.

Homogeneous linewidth narrowing of the charged exciton via nuclear spin screening in an InAs/GaAs quantum dot ensemble

In semiconductor quantum dots, the electron hyperfine interaction with the nuclear spin bath is the leading source of spin decoherence at cryogenic temperature. Using high-resolution two-color differential transmission spectroscopy, we demonstrate that such electron-nuclear coupling also imposes a lower limit for the positively charged exciton dephasing rate, \gamma, in an ensemble of InAs/GaAs quantum dots. We find that the dephasing rate is sensitive to the strength of the hyperfine interaction, which can be controlled through the application of an external magnetic field in the Faraday configuration. At zero applied field, strong electron-nuclear coupling induces additional dephasing beyond the radiative limit and \gamma = 230 MHz (0.95 \mu eV). Screening of the hyperfine interaction is achieved for an external field of ~1 T, resulting in \gamma = 172 MHz (0.71 \mu eV) limited only by spontaneous recombination. On the other hand, application of a Voigt magnetic field mixes the spin eigenstates, which increases the dephasing rate by up to 75%. These results are reproduced with a simple and intuitive model that captures the essential features of the electron hyperfine interaction and its influence on \gamma.

Microscopic model for intersubband gain from electrically pumped quantum-dot structures

We study theoretically the performance of electrically pumped self-organized quantum dots as a gain material in the mid-IR range at room temperature. We analyze an AlGaAs/InGaAs based structure composed of dots-in-a-well sandwiched between two quantum wells. We numerically analyze a comprehensive model by combining a many-particle approach for electronic dynamics with a realistic modeling of the electronic states in the whole structure. We investigate the gain both for quasi-equilibrium conditions and current injection. Comparing different structures we find that steady-state gain can only be realized by an efficient extraction process, which prevents an accumulation of electrons in continuum states, that make the available scattering pathways through the quantum dot active region too fast to sustain inversion. The tradeoff between different extraction/injection pathways is discussed. Comparing the modal gain to a standard quantum-well structure as used in quantum cascade lasers, our calculations predict reduced threshold current densities of the quantum dot structure for comparable modal gain. Such a comparable modal gain can, however, only be achieved for an inhomogeneous broadening of a quantum-dot ensemble that is close to the lower limit achievable today using self-organized growth.

Anomalous spectral dependence of optical polarization and its impact on spin detection in InGaAs/GaAs quantum dots

We show that circularly polarized emission light from InGaAs/GaAs quantum dot (QD) ensembles under optical spin injection from an adjacent GaAs layer can switch its helicity depending on emission wavelengths and optical excitation density. We attribute this anomalous behavior to simultaneous contributions from both positive and negative trions and a lower number of photo-excited holes than electrons being injected into the QDs due to trapping of holes at ionized acceptors and a lower hole mobility. Our results call for caution in reading out electron spin polarization by optical polarization of the QD ensembles and also provide a guideline in improving efficiency of spin light emitting devices that utilize QDs.

Comparison of gain and phase recovery dynamics among optical pumping schemes in quantum-dot semiconductor optical amplifiers

We numerically compare the gain and phase recovery acceleration of quantum-dot (QD) semiconductor optical amplifiers (SOAs) caused by four optical pumping schemes: the single-color optical pumping tune to the quantum-well (QW) carrier reservoir; the QD excited state (ES) ensembles; and the QD ground state (GS) ensembles together with multicolor optical pumping tuned to the GS and ES ensembles of QDs. The temporal responses of the gain and phase recoveries caused by the four optical pumping schemes are calculated and compared by solving 1088 coupled rate equations at the same pumping conditions. Among the four optical pumping schemes, the single-color optical pumping to the ES ensemble shows the fastest response of the gain and phase recovery. This results from the large carrier occupation ratio at the GS and ES ensembles and the high modal gain at the pumping wavelength, which facilitates the reduction of the carrier recovery time within the GS and ES ensembles due to the increased stimulated recombination rate caused by the optical pumping beam.

Two-colour spin noise spectroscopy and fluctuation correlations reveal homogeneous linewidths within quantum-dot ensembles.

'Spin noise spectroscopy' is an optical technique for probing electron and hole spin dynamics that is based on detecting their intrinsic fluctuations while in thermal equilibrium. Here we show that fluctuation correlations can be further exploited in multi-probe noise studies to reveal information that in general cannot be accessed by conventional linear optical spectroscopy, such as the underlying homogeneous linewidths of individual constituents within inhomogeneously broadened systems. This is demonstrated in singly charged (In,Ga)As quantum-dot ensembles using two weak probe lasers: When the lasers have similar wavelengths, they probe the same quantum dots in the ensemble and show correlated spin fluctuations. In contrast, mutually detuned probe lasers measure different subsets of quantum dots, giving uncorrelated fluctuations. The noise correlation versus laser detuning directly reveals the quantum dot homogeneous linewidth even in the presence of a strong inhomogeneous broadening. Such noise-based correlation techniques are not limited to semiconductor spin systems, but are applicable to any system with measurable intrinsic fluctuations.

Superradiance and enhanced luminescence from ensembles of a few self-assembled quantum dots

We study the evolution of photoluminescence (PL) from homogeneous and inhomogeneous ensembles of a few coupled QDs. We discuss the relation between signals from a given QD ensemble under strong and weak excitation (full inversion and linear response regimes): A system homogeneous enough to manifest superradiant emission when strongly inverted shows a non-exponential decay of the PL signal under spatially coherent weak excitation. In an inhomogeneous ensemble the PL decay is always nearly exponential with a qualitatively different form of the time dependence in the two excitation regimes and with a higher rate under weak excitation.

Quantum-size-controlled photoelectrochemical fabrication of epitaxial InGaN quantum dots.

We demonstrate a new route to the precision fabrication of epitaxial semiconductor nanostructures in the sub-10 nm size regime: quantum-size-controlled photoelectrochemical (QSC-PEC) etching. We show that quantum dots (QDs) can be QSC-PEC-etched from epitaxial InGaN thin films using narrowband laser photoexcitation, and that the QD sizes (and hence bandgaps and photoluminescence wavelengths) are determined by the photoexcitation wavelength. Low-temperature photoluminescence from ensembles of such QDs have peak wavelengths that can be tunably blue shifted by 35 nm (from 440 to 405 nm) and have line widths that narrow by 3 times (from 19 to 6 nm).

Growth-temperature dependence of optical spin-injection dynamics in self-assembled InGaAs quantum dots

The growth-temperature dependence of the optical spin-injection dynamics in self-assembled quantum dots (QDs) of In0.5Ga0.5As was studied by increasing the sheet density of the dots from 2 × 1010 to 7 × 1010 cm−2 and reducing their size through a decrease in growth temperature from 500 to 470 °C. The circularly polarized transient photoluminescence (PL) of the resulting QD ensembles was analyzed after optical excitation of spin-polarized carriers in GaAs barriers by using rate equations that take into account spin-injection dynamics such as spin-injection time, spin relaxation during injection, spin-dependent state-filling, and subsequent spin relaxation. The excitation-power dependence of the transient circular polarization of PL in the QDs, which is sensitive to the state-filling effect, was also examined. It was found that a systematic increase occurs in the degree of circular polarization of PL with decreasing growth temperature, which reflects the transient polarization of exciton spin after spin injection. This is attributed to strong suppression of the filling effect for the majority-spin states as the dot-density of the QDs increases.

Excitation of complex spin dynamics patterns in a quantum-dot electron spin ensemble

We exploit the flexibility offered by an (In,Ga)As/GaAs quantum dot spin ensemble to demonstrate that complex dynamic evolutions can be excited in the ensemble magnetization and accessed by tailored pulsed laser protocols. The modes for spin precession about a magnetic field are adapted to the periodic excitation protocol such that at specific times the magnetization can effectively be decomposed in two, three, or four equal components with angles of $\ensuremath{\pi},2\ensuremath{\pi}/3$, or $\ensuremath{\pi}/2$ between them. Optical orientation of these components by an additional laser pulse leads to the generation of higher harmonics in the spin precession, as evidenced by time-resolved ellipticity measurements.

Absorption spectra of CdSe–ZnS core–shell quantum dots at high photon energies: Experiment and modeling

Absorption spectra of CdSe–ZnS core–shell quantum dot (QD) ensembles, with average core diameters ranging from 2.6nm to 7.2nm have been obtained using both transmission and photoluminescence excitation measurements. In agreement with previous reports, the absorption coefficient at energies ≃1eV above the effective bandgap increases monotonically as in bulk solids. A simple effective-mass spherical core–shell potential model cannot explain the relatively high absorption at higher energies. The calculated electron and hole radial envelope wavefunctions show asymmetry due to the core–shell structure. It leads to normally symmetry-disallowed transitions acquiring a weak oscillator strength, with their number and strength increasing with energy. A phenomenological model that invokes normally disallowed transitions in general is shown to reproduce the absorption spectrum at higher energies quite well. The oscillator strength scaling factor for such transitions increases with decrease in QD size, consistent with expectations.

Stark effect in ensembles of polar (0001) Al0.5Ga0.5N/GaN quantum dots and comparison with semipolar (11−22) ones

This work presents a continuous-wave photoluminescence study of Al0.5Ga0.5N/GaN quantum dots grown by ammonia-assisted molecular beam epitaxy on sapphire, either on the wurtzite polar (0001) or the semipolar (11−22) plane. Due to interface polarization discontinuities, the polar dots are strongly red-shifted by the Stark effect and emit in the visible range. Carrier injection screening of the polarization charges has been studied. A model relying on average dot heights and dot height variances, as measured by transmission electron microscopy, is proposed. It can account for the injection dependent luminescence energies and efficiencies. The electric field discontinuity deduced from the fittings is in good agreement with theoretical expectations for our barrier composition. On the contrary, semipolar quantum dot ensembles always emit above the gap of GaN strained to Al0.5Ga0.5N. Their luminescence linewidth is significantly lower than that of polar ones, and their energy does not shift with injection. Our study then confirms the expected strong decrease of the Stark effect for (11−22) grown (Al,Ga)N/GaN heterostructures.