Analysis of the modified optical properties and band structure of GaAs12xSbx-capped InAs/GaAs quantum dots

The origin of the modified optical properties of InAs/GaAs quantum dots (QD) capped with a thin GaAs1−xSbx layer is analyzed in terms of the band structure. To do so, the size, shape, and composition of the QDs and capping layer are determined through cross-sectional scanning tunnelling microscopy and used as input parameters in an 8 × 8 k·p model. As the Sb content is increased, there are two competing effects determining carrier confinement and the oscillator strength: the increased QD height and reduced strain on one side and the reduced QD-capping layer valence band offset on the other. Nevertheless, the observed evolution of the photoluminescence (PL) intensity with Sb cannot be explained in terms of the oscillator strength between ground states, which decreases dramatically for Sb > 16%, where the band alignment becomes type II with the hole wavefunction localized outside the QD in the capping layer. Contrary to this behaviour, the PL intensity in the type II QDs is similar (at 15 K) or even larger (at room temperature) than in the type I Sb-free reference QDs. This indicates that the PL efficiency is dominated by carrier dynamics, which is altered by the presence of the GaAsSb capping layer. In particular, the presence of Sb leads to an enhanced PL thermal stability. From the comparison between the activation energies for thermal quenching of the PL and the modelled band structure, the main carrier escape mechanisms are suggested. In standard GaAs-capped QDs, escape of both electrons and holes to the GaAs barrier is the main PL quenching mechanism. For small-moderate Sb (<16%) for which the type I band alignment is kept, electrons escape to the GaAs barrier and holes escape to the GaAsSb capping layer, where redistribution and retraping processes can take place. For Sb contents above 16% (type-II region), holes remain in the GaAsSb layer and the escape of electrons from the QD to the GaAs barrier is most likely the dominant PL quenching mechanism. This means that electrons and holes behave dynamically as uncorrelated pairs in both the type-I and type-II structures.

High optical sensitivity to ambient conditions of uncapped InGaAs surface quantum dots

The influence of the environment on the optical properties of self-assembled In0.5Ga0.5As surface quantum dots is studied as a function of different ambient conditions for sensing applications. Their room temperature photoluminescence (PL) quenches under vacuum and decreases strongly under dry O2 or N2 environments. Nevertheless, they have a strong signal at 1.55 lm in air or in a wet atmosphere. The presence of water molecules in the environment improves the PL intensity likely due to its polar character and therefore its easier adsorption by the surface dangling bonds, leading to a suppression of the non-radiative recombination centers.

Effect of Sb incorporation on the electronic structure of InAs quantum dots

On the basis of optical characterization experiments and an eight band kp model, we have studied the effect of Sb incorporation on the electronic structure of InAs quantum dots (QDs). We have found that Sb incorporation in InAs QDs shifts the hole wave function to the center of the QD from the edges of the QD where it is otherwise pinned down by the effects of shear stress. The observed changes in the ground-state energy cannot merely be explained by a composition change upon Sb exposure but can be accounted for when the change in lateral size is taken into consideration. The Sb distribution inside the QDs produces distinctive changes in the density of states, particularly, in the separation between excitation shells. We find a 50% increase in the thermal escape activation energy compared with reference InAs quantum dots as well as an increment of the fundamental transition decay time with Sb incorporation. Furthermore, we find that Sb incorporation into quantum dots is strongly nonlinear with coverage, saturating at low doses. This suggests the existence of a solubility limit of the Sb incorporation into the quantum dots during growth.

Self-organized colloidal quantum dots and metal nanoparticles for plasmon-enhanced intermediate-band solar cells

A colloidal deposition technique is presented to construct long-range ordered hybrid arrays of self-assembled quantum dots and metal nanoparticles. Quantum dots are promising for novel opto-electronic devices but, in most cases, their optical transitions of interest lack sufficient light absorption to provide a significant impact in their implementation. A potential solution is to couple the dots with localized plasmons in metal nanoparticles. The extreme confinement of light in the near-field produced by the nanoparticles can potentially boost the absorption in the quantum dots by up to two orders of magnitude. In this work, light extinction measurements are employed to probe the plasmon resonance of spherical gold nanoparticles in lead sulfide colloidal quantum dots and amorphous silicon thin-films. Mie theory computations are used to analyze the experimental results and determine the absorption enhancement that can be generated by the highly intense near-field produced in the vicinity of the gold nanoparticles at their surface plasmon resonance. The results presented here are of interest for the development of plasmon-enhanced colloidal nanostructured photovoltaic materials, such as colloidal quantum dot intermediate-band solar cells.

Effect of field damping layer on two step absorption of quantum dots solar cells

Multi-stacked InAs/AlGaAs quantum dot solar cells (QDSCs) introduced with field damping layers (FDL) which sustain the junction built-in potential have been studied. Without an external bias condition, the external quantum efficiency (EQE) of QD layers are reduced by introducing the thick FDL, because the carrier escape due to built-in electric field was suppressed. On the other hand, the photocurrent production due to two-step absorption is increased by the formation of flat-band QD structure for QDSC with thick FDL.

Stacked GaAs(Sb)(N)-capped InAs/GaAs quantum dots for enhanced solar cell efficiency

Different approaches have arisen aiming to exceed the Shockley-Queisser efficiency limit of solar cells. Particularly, stacking QD layers allows exploiting their unique properties, not only for intermediate-band solar cells or multiple exciton generation, but also for tandem cells in which the tunability of QD properties through the capping layer (CL) could be very useful.

Stacked GaAsSbN-capped InAs/GaAs quantum dots for enhanced solar cell efficiency

Different approaches have recently arisen aiming to exceed the Shockley-Queisser efficiency limit. Particularly, the use of self-organized quantum dots (QD) has been recently proposed in order to introduce new states within the barrier material, which enhances the subband gap absorption yielding a photocurrent increase. Stacking QD layers allows exploiting their unique properties for intermediate-band solar cells (SC) or tandem cells.In all these cases, tuning the QD properties by modifying the capping layer (CL) can be very useful.

Height control of self-assembled quantum dots

The capping of epitaxially grown Quantum Dots (QD) is a key process in the fabrication of devices based on these nanostructures because capping can significantly affect the QDs morphology [3]. We have studied the QD morphology after capping in order to better understand the role of the capping process. We have grown real structures and compared the QD morphology obtained by cross-sectional Scanning Tunneling Microscopy (X-STM) with the morphology of QDs that were virtually grown in simulations based on a Kinetic Monte Carlo model (KMC) [1].

Tunable Raman photons in singly charged p-doped quantum dots

The obtention of spontaneous Raman photons is analyzed in singly charged p-doped quantum dots in the absence of an external magnetic field. The use of a far detuned single driving laser allows to obtain a Raman photon line which exhibits subnatural linewidth, and whose center can be tuned by changing the detuning and/or the Rabi frequency of the driving field. The Raman photons are produced along the undriven transition and they arise from the weak interaction of the trion states with the nuclear spins. The operating point for the gate voltage of the heterostructure can also be used to modify the linewidth and the peak value of the fluorescent signal.

Fano-Rashba effect in quantum dots

We consider the electronic transport through a Rashba quantum dot coupled to ferromagnetic leads. We show that the interference of localized electron states with resonant electron states leads to the appearance of the Fano-Rashba effect. This effect occurs due to the interference of bound levels of spin-polarized electrons with the continuum of electronic states with an opposite spin polarization. We investigate this Fano-Rashba effect as a function of the applied magnetic field and Rashba spin-orbit coupling.

Single-exciton spectroscopy of semimagnetic quantum dots

A photoexcited II-VI semiconductor quantum dots doped with a few Mn spins is considered. The effects of spin-exciton interactions and the resulting multispin correlations on the photoluminescence are calculated by numerical diagonalization of the Hamiltonian, including exchange interaction between electrons, holes, and Mn spins, as well as spin-orbit interaction. The results provide a unified description of recent experiments on the photoluminesnce of dots with one and many Mn atoms as well as optically induced ferromagnetism in semimagnetic quantum dots.

Spin-phonon coupling in single Mn-doped CdTe quantum dot

The spin dynamics of a single Mn atom in a laser driven CdTe quantum dot is addressed theoretically. Recent experimental results [ Gall et al. Phys. Rev. Lett. 102 127402 (2009);  Goryca et al. Phys. Rev. Lett. 103 087401 (2009)  Gall et al. Phys. Rev. B 81 245315 (2010)] show that it is possible to induce Mn spin polarization by means of circularly polarized optical pumping. Pumping is made possible by the faster Mn spin relaxation in the presence of the exciton. Here we discuss different Mn spin-relaxation mechanisms: first, Mn-phonon coupling, which is enhanced in the presence of the exciton; second, phonon induced hole spin relaxation combined with carrier-Mn spin-flip coupling and photon emission results in Mn spin relaxation. We model the Mn spin dynamics under the influence of a pumping laser that injects excitons into the dot, taking into account exciton-Mn exchange and phonon induced spin relaxation of both Mn and holes. Our simulations account for the optically induced Mn spin pumping.

Transport across two interacting quantum dots: Bulk Kondo, Kondo box, and molecular regimes

We analyze the transport properties of a double quantum dot device with both dots coupled to perfect conducting leads and to a finite chain of N noninteracting sites connecting both of them. The interdot chain strongly influences the transport across the system and the local density of states of the dots. We study the case of a small number of sites, so that Kondo box effects are present, varying the coupling between the dots and the chain. For odd N and small coupling between the interdot chain and the dots, a state with two coexisting Kondo regimes develops: the bulk Kondo due to the quantum dots connected to leads and the one produced by the screening of the quantum dot spins by the spin in the finite chain at the Fermi level. As the coupling to the interdot chain increases, there is a crossover to a molecular Kondo effect, due to the screening of the molecule (formed by the finite chain and the quantum dots) spin by the leads. For even N the two Kondo temperatures regime does not develop and the physics is dominated by the usual competition between Kondo and antiferromagnetism between the quantum dots. We finally study how the transport properties are affected as N is increased. For the study we used exact multiconfigurational Lanczos calculations and finite-U slave-boson mean-field theory at T=0. The results obtained with both methods describe qualitatively and also quantitatively the same physics.

Theory of many-particle correlations and optical properties of semiconductor quantum dots : photons and quantum dots

Otto-von-Guericke-Universität Magdeburg, Fakultät für Naturwissenschaften, Dissertation, 2016