Dynamics and coherent effects on high density plasmas in semiconductor nanostructures

This thesis work contains an experimental study of many-body and cooperative effects in quantum wells. Many-body effects prove important for an understanding of the physical and specifically optical properties of semiconductors. The Coulomb interaction between electrons profoundly modifies the electronic states and the light-matter interaction, leading to a number of density-dependent effects that can not be accounted for in the one-electron picture which is the starting point of most textbooks on the subject. The simplest of these modifications is the exciton, the bound state of one electron and one hole which leads to the emergence of two-particle states energetically below the continuous band electron-hole states. Optical excitation in the band continuum is possibly followed by the formation of excitons upon release of the excess energy to the lattice vibrations. Chapter 5 contains an experimental analysis of the dynamics of this process. A high quality single In0.05Ga0.95As/GaAs quantum well sample allows us to separately study the temporal evolution of the continuum photoluminescence on the one hand and the excitonic photoluminescence on the other. The results indicate a rather fast formation process, leading to the establishment of a species interconversion equilibrium between free pairs and bound pairs at higher density. However, at the lowest excitation density, we found evidence for a non-equilibrium species repartition. At high electron-hole pair density, the two-particle bound exciton state disappears due to the screening of the Coulomb interaction by the surrounding carriers as well as the blocking of the constituting states according to the Pauli exclusion principle. The transition from an excitonic population to a free carrier plasma is referred to as excitonic Mott transition. Chapter 6 reports an experimental investigation of the repercussions of this transition on the optical spectra, performed on the In0.05Ga0.95As/GaAs quantum well of chapter 5. The time-resolved spectra do not show an abrupt change of photoluminescence intensity or spectral form when transforming gradually from an exciton dominated spectrum to free plasma photoluminescence, indicating a rather gradual transition. The separate visibility of continuum and excitonic PL contributions below the transition density reveals the total absence of exciton binding energy variations, indicating a very low exciton ionization degree in contrast to theoretical work on the subject. Another high-density effect arising from the particle interactions is the energetic lowering of the electronic states due to screening and correlation, denoted as band gap renormalization (BGR). Chapter 7 presents measurements of BGR using a single GaAs/Al0.25Ga0.75As quantum well of 60 Å width. We obtain good agreement with calculations of the carrier self energy within the framework of the random phase approximation. The last part of this thesis (chapter 8) reports an experimental test of the possibility of cooperative spontaneous emission, often denoted as superradiance, from a high-density electron-hole plasma. This effect has been extensively studied in optically excited atomic gases, where it leads under certain conditions to the reemission of the stored energy in a single coherent radiation burst instead of the slow exponential decay according to the spontaneous radiation of a single atom. We find no evidence for the occurrence of this effect in our samples, probably due to the fast incoherent polarization decay in the carrier plasma.

Tailored-Potential Pyramidal Quantum Dot Heterostructures

Valentina Troncale

Semiconductor quantum dots are usually compared to artificial atoms, because their electronic structure consists of discrete energy levels as for natural atoms. These artificial systems are integrated in solid materials and can be localized with a spatial precision of the order of nanometers. Besides, they conserve their quantum properties even at quite high temperatures (∼ 10 K). These properties make quantum dots one of the most suitable systems for the realization of quantum devices and computers. However, the energy states and the optical properties of quantum dots are much more complicated than for atoms, because a quantum dot is never an isolated potential well. Instead, its electronic structure depends on the crystallin structure of the semiconductor material and on the Coulomb ion-electron and electron-electron correlations. In particular, the presence of several valence bands and their mixing, induced by quantum confinement, gives rise to novel properties which are still not completely understood and exploited in applications. To get a major advance in this field, a full deterministic control of the spatial shape of the quantum confinement is needed, combined with a deeper understanding of the connections between electronic and optical properties. This thesis work has these two main objectives. We realized and experimentally studied different quantum dot systems, in pyramidal hetero-structures grown with MOCVD techniques. These systems allowed the realization of several different geometries for the carrier confining potential, with a precision in the order of nanometers. The optical characterization has been obtained in particular by means of polarization-resolved microphotoluminescence, magneto-photoluminescence, excitation photoluminescence (PLE), and interferometry techniques. For single quantum dots, we have observed and characterized for the first time new excitonic complexes, arising from excited hole states. This allowed a full caracterizatioon of the valence band hole states in our peculiar system. By means of photon correlation measurements, we have also experimentally demonstrated that, even in presence of a large family of exciton states, these quantum dot systems can emit single photons. We have then realized much more complex quantum dot structures, double dot systems (quantum dot molecules) and a completely new system called Dot-in-Dot (DiD). This latter is composed by a small inner dot surrounded by an electrostatic potential well (which can be considered as an outer elongated dot). Such a composite system is characterized by a strong valence band mixing. This state superposition is however very sensitive to small variations of the confining potential. Therefore the degree of valence band mixing can be easily switched by the introduction of a week external field. Since the valence band mixing determines the polarization properties of the emitted light, the DiD changes the polarization properties of its emission spectrum under the action of an external field. In particular, we have experimentally demonstrated this effect for an external static magnetic field, while we have numerically predicted a very similar effect for a static electric field. In the latter case, the polarization switching is a direct consequence of the quantum confined Stark effect induced in the DiD. Hence the DiD appears to be an ideal candidate for realizing emitters of single photons with tunable and controllable polarization.

EPFL2010

Dynamics of quantum dot lasers

Pablo Moreno

The exceptional performance of self-assembled Quantum Dot (QD) materials renders them extremely appealing for their use as optical communications devices. As lasers, they feature reduced and temperature independent threshold current and proper emission wavelength at the fiber telecommunication windows. These characteristics, together with the low linewidth enhancement factor and broad spectrum, make QD materials extremely attractive for application as light emitters or amplifiers. There exist, nevertheless, several unclear issues which prevent QDs from conquering the new generation of optoelectronic devices. Their differential efficiency is lower than expected. The output power of QD lasers is lower than that of their quantum well counterpart. Still, it is their dynamics which has incited the majority of studies. The modulation bandwidth of these devices seems to be limited by the relaxation of carriers from the upper energetic layers to the low levels within the dot. Besides, the electron-hole interaction is widely unknown, the extent of the electron-hole Coulombic attraction is not yet established. Throughout this thesis I present a theoretical and experimental study of the gain and phase dynamics of quantum dot lasers. I explain the appearance of different decay times observed in pump and probe experiments in QD amplifiers as a result of the different electron and hole relaxation times, by means of an electron-hole rate-equation model. The ultrafast hole relaxation first leads to an ultrafast recovery of the gain, which is then followed by electron relaxation and, on the nanosecond timescale, radiative and non-radiative recombinations. The phase dynamics is slower and is affected by thermal redistribution of carriers within the dot. Our results corroborate with spectral measurements of the dephasing and gain in QD amplifiers. Additionally, our work is compared with existing pump and probe results. Exploiting the capacity of QD lasers to emit at two different wavelengths corresponding to the ground state (GS) and excited state (ES), I present a theoretical study of the QD dynamics, based on a linearization of the QD rate-equations. The results predict the existence of single oscillation frequency of GS and ES, meaning that both states are highly coupled. In order to verify our theory, we perform two kinds of experiments. By modulating these lasers at high frequency, we measure separately the dynamics of GS and ES. However, in contradiction to our theory, two different modulation frequencies are found. Additional temporally-resolved measurements of the laser dynamics reveal a surprising effect. By injecting a sub-bandgap pump in an InAs/InGaAs QD laser, the emitted photons are depleted. Through additional transmission and photocurrent measurements, we relate this observation with carrier photoexcitation, which was so far only theoretically addressed. The role of carrier photoexcitation in our experimental laser dynamics is further supported by a rate-equation model. Impelled by this finding, we study the effect of carrier photoexcitation in the static and dynamic characteristics. We find that carrier photoexcitation reduces the efficiency of QD lasers, which is one of the major QD handicaps, and depletes the GS lasing after the ES threshold, as observed experimentally. Moreover, by adding carrier photoexcitation to our linearization of the rate-equations, we find that the theory predicts the appearance of two lasing resonance frequencies, in agreement with our previous experimental results. Additionally, we deal with the improvement of carrier relaxation. In tunnel injection devices, carriers are given an additional path towards the ground state of the dot by growing a quantum well layer close to the QD active plane. Through the quantum-mechanical tunneling effect, carriers relax from the nearby quantum well layer to the QDs, which speeds up relaxation. We aim at the increase of the modulation bandwidth while keeping the good performances quantum dot lasers have exhibited, such as low and temperature insensitive threshold current and proper emission wavelength. In the final part of this work, we present dynamical measurements of 1.5 µm InAs/InP tunnel injection and non-tunnel injection QD lasers, which display remarkable static characteristics. After proving with static measurements that tunnel injection is actually taking place in these structures, we show several dynamic measurements. Pump and probe measurements on QD devices show that the tunnel injection samples exhibit a slightly faster relaxation time than the non-tunnel injection samples used as reference, meaning that relaxation time is improved with tunnel injection. However, by probing the device with an ultrafast pump no improvement of the dynamic characteristics is observed. These results confirm that the laser dynamic properties of InP QD lasers, both standard and tunnel-injection designs, are actually not limited by relaxation of carriers. We point towards the size distribution of these quantum dash-like structures as the limiting factor of the modulation frequency.

EPFL2008

Ab initio study of interface states at metal contacts to III-IV semiconductors

Thomas Maxisch

We present a theoretical study of the physical characteristics of metal/semiconductor junctions. Using first principle pseudopotential calculations, we have investigated the nature of electronic states with energies within the semiconductor band gap of representative abrupt, defect-free, anion-terminated metal/III-V interfaces. Namely, we focused on Al contacts to GaAs(001), AlAs(001) and cubic GaN(001) as well as on Al, Au and Cu junctions to cubic GaN(001). Recent advances in Schottky barrier concepts emphasize the possible relationship between interface states and the formation of the Schottky barrier. We aim at understanding the atomic-scale mechanisms responsible for interface states as well as their role in the Schottky barrier formation process. At As-terminated Al/GaAs(001) and Al/AlAs(001) junctions, resonant and localized interface states occur at the J point of the interface 2D Brillouin zone near the Fermi energy in the semiconductor midgap region. They correspond to intermetallic bonds between the outermost cation atoms of the semiconductor and the interfacial Al atoms of the metal. These interface states derive from an interaction between localized states of the Al(001) surface and semiconductor conduction band states, mediated by localized states of the unreconstructed, As-terminated semiconductor (001) surface. Our results indicate that interface states of the intermetallic, bonding-like kind could play an important role in the transport properties of metal/AlxGa1-xAs junctions. We have also investigated the electronic structure of Al, Au and Cu junctions to cubic, N-terminated GaN(001). The localized interface state reported for As-terminated Al/GaAs(001) and Al/AlAs(001) junctions occurs also at metal/GaN interfaces under the condition that atoms on the outermost atomic plane of the metal are placed in front of the outermost semiconductor cation. This indicates that the formation mechanism of this state is a very general one. In contrast to Al/AlxGa1-xAs junctions, these states occur at energy much larger than EF for the contacts to GaN. Thus, they are not expected to contribute significantly to the electronic transport of the latter interfaces. However, a large number of interface states attributed to d-type orbitals occur over a wide energy range including EF at contacts of noble metals to GaN.

EPFL2003