Quantum dot

Summary

Quantum dots (QDs) – also called semiconductor nanocrystals, are semiconductor particles a few nanometres in size, having optical and electronic properties that differ from those of larger particles as a result of quantum mechanics. They are a central topic in nanotechnology and materials science. When the quantum dots are illuminated by UV light, an electron in the quantum dot can be excited to a state of higher energy. In the case of a semiconducting quantum dot, this process corresponds to the transition of an electron from the valence band to the conductance band. The excited electron can drop back into the valence band releasing its energy as light. This light emission (photoluminescence) is illustrated in the figure on the right. The color of that light depends on the energy difference between the conductance band and the valence band, or the transition between discrete energy states when the band structure is no longer well-defined in QDs. Nanoscale semiconductor materials t

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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

Optically active quantum dots in bottom-up nanowires

Yannik Fontana

This thesis is dedicated to the discovery and progressive study of quantum emitters embedded in the shell of coaxial gallium arsenide/ aluminum gallium arsenide nanowires. The bottom-up core/shell nanowires were grown in a molecular beam epitaxy machine. During the shell growth, diffusion-driven phenomena lead to segregation effects. Gallium-rich regions are formed at the nanoscopic scale. The observation has been made that the reduced dimensionality of these regions provides true tridimensional confinement for the carriers. The recombination spectra of the electrons with the holes in what was coined shell quantum dots (shell-QDs) thus appear as sets of narrow, intense peaks. The formation of shell quantum dots is taking place on a large range of growth temperatures and nominal alloy fractions, giving freedom to engineer the growth process. The shell thickness plays an important role in the quantum dot density and total ensemble spectrum. In addition, the adjunction of an aluminum arsenide predeposition layer increasing the local curvature has been seen to foster the quantum dots formation. Single emitter spectroscopy reveals the few-particles electronic structure of quantum dots, with systematic signatures for the different degrees of occupation of the quantum dot. The shape anisotropy of the quantum dots leads to observable spin-spin interactions, which lift the degeneracy of the exciton level (one hole and one electron). Generally undesirable, this effect allows here to find that the orientation of the quantum dots in the nanowire is not hard-wired to the growth direction or to the nanowire long axis. This observation is confirmed by magneto-photoluminescence experiments. The energetic splitting and shift of the spin sublevels when an external magnetic field is applied also confirms the small size of the quantum dots. It is found that for GaAs in the strong confinement regime, the Landé coefficients of the electron and hole take opposite signs and are dependent on the angle at which the field is applied. These effects allow to tune the exciton composite Landé coefficient and could be used to reduce the splitting between the exciton spin sublevels or create optically degenerate coupled systems. Finally, the sub-nanosecond dynamics happening in the quantum dots are probed with time-correlated photon counting. It is shown that the carriers in the shell are quickly captured by the quantum dots. In addition, it is proposed that the electron population is reduced due to diffusion-assisted mechanisms or through electron-donor recombination.

EPFL2015

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