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Investigating the Factors Governing the Efficiency and the Electroluminescence Stability in Simplified Phosphorescent Organic Light-Emitting Devices Utilizing One Material for Both Hole Transport and Emitter HostAbdelmalek, Mina 10 December 2013 (has links)
Organic Light-Emitting Devices (OLEDs) have reached industrial maturity in display technology, since OLEDs provide salient advantages such as high brightness, fast response, wide viewing angle, mechanical flexibility, and low cost manufacturing. Due to the ability of electroluminescence (EL) from triplet excited states as well as singlet excited states, phosphorescent OLEDs (PHOLEDs) have a potential to achieve 100% internal quantum efficiency. Therefore, PHOLEDs can offer a competitive external quantum efficiency. However, the operational stability of PHOLEDs is relatively poor. Several mechanisms have been proposed to address the chemical and physical phenomena associated with intrinsic degradation of PHOLEDs, nevertheless, the reasons behind voltage rise and luminance loss accompanying PHOLEDs long term operation are not yet well understood. The state of the art p-i-n PHOLEDs offer relatively high efficiency and low efficiency roll-off. However, this technology is characterized by structure complexity. Therefore, much of the current research on PHOLEDs focuses on the development of the simplest possible and most easily processed architecture that can deliver the optimal combination of device properties. Simplified PHOLEDs, utilizing one material for both hole transport and emitter host, can be a good candidate for replacement of p-i-n technology. Simplified PHOLEDs offer higher efficiency than the p-i-n PHOLEDs , yet, their EL stability is found to be poor.
In this thesis, the role of the ITO/organic interface on simplified PHOLEDs efficiency will be investigated. Furthermore, possible degradation mechanisms at the ITO/organic interface will be explored. Moreover, we will correlate degradation at the ITO/organic interface to PHOLEDs operational stability. Eventually, organic layers modifications including but not limited to emissive layer (EML) will be examined.
By studying the indium tin oxide (ITO)/organic interface in simplified PHOLEDs, it was found that this interface is critical to PHOLEDs performance. The study shows that, this interface is critical to the PHOLED overall stability and is considered as one of the limiting factors of the long term operational stability of simplified PHOLEDs. The effect of optical excitation on the ITO/organic interface stability in hole-only devices was investigated. It was found that the ITO/organic interface is susceptible to exciton-induced degradation. This degradation affects the device stability severely compared to current-induced degradation. The exciton-induced degradation can be prevented by doping the hole transport layer (HTL), at the interface with an exciton quencher layer or by blocking the electrons from leaking to the ITO/organic interface that may further recombine with holes to form excitons. Further studies showed that upon combining both electrical stress and optical excitation, the device degradation is even more pronounced which is most likely due to interactions between charges and excitons. By using exciton life-time measurements, a new role of molybdenum trioxide (MoO3) in the electrical stability of PHOLEDs, as an exciton quencher layer, is introduced.
Delayed EL (DEL) measurements showed that the simplified PHOLEDs are susceptible to triplet-triplet annihilation (TTA) and triplet-polaron quenching (TPQ) which might affect the operational stability of simplified PHOLEDs. Finally, EML modifications showed that the recombination zone of simplified PHOLEDs is located near the HTL/EML interface.
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Time-integrated and time-resolved optical studies of InGaN quantum dotsRobinson, James W. January 2005 (has links)
The construction of a high-resolution optical microscope system for micro-photoluminescence (µ-PL) spectroscopy is described, and a range of time-integrated and time-resolved experimental work on single InGaN quantum dots (QDs) is presented. Time-integrated measurements demonstrate the existence of InGaN QDs in three different samples via the presence of sharp exciton recombination lines in the µ-PL spectra. The narrowest peaks display a linewidth Γ of ~230 µeV, implying a decoherence time T2 ≥5.7 ps. Time-resolved measurements on exciton recombination lines from single self-assembled InGaN QDs reveal typical lifetimes of ~2.0 ns (which decrease with increasing temperature), while typical lifetimes for excitons in single selectively-grown micropyramidal InGaN QDs are found to be ~0.4 ns. The shorter exciton recombination lifetime in selectively-grown QDs is believed to be due to a stronger coupling of these QDs to the underlying quantum well. Temporal fluctuations (on a timescale of seconds) in the energy, intensity and FWHM of µ-PL peaks arising from the recombination of excitons in single self-assembled InGaN QDs are observed. These are attributed to transient Stark shifts induced by a fluctuating local charge distribution as carriers become trapped in defect states in the vicinity of the QDs. Time-integrated power-dependent measurements are used to demonstrate the presence of biexciton states in single self-assembled InGaN QDs. The exciton–biexciton energy splitting is found to be ~41 meV, in agreement with values predicted by theoretical calculations. Time-resolved studies of the biexciton and exciton decay curves reveal a coupling as the exciton population is refilled by biexciton decays. The biexciton lifetime is found to be ~1.4 ns, compared to an exciton lifetime of ~1.0 ns. Lateral electric fields are applied to a single self-assembled InGaN QD using aluminium electrodes lithographically defined on the sample surface. Application of fields of the order of ~0.17 MVcm-1 is found to cause both a red-shift and a reduction in the intensity of the exciton recombination peak in the µ-PL spectrum.
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Manipulation cohérente de l'émission résonnante d'une boîte quantique uniqueTonin, Catherine 21 September 2012 (has links) (PDF)
Le but de cette thèse a été de mettre en évidence notre capacité à utiliser des boîtes quantiques semi-conductrices comme support à la réalisation de bits quantiques, briques élémentaires de l'information quantique. Nous avons ainsi démontré la possibilité de définir un système à deux niveaux, dont l'initialisation et le contrôle est réalisable au moyen d'impulsions lumineuses picosecondes et déterminé le temps durant lequel nous étions en mesure de conserver sa cohérence. Les oscillations de Rabi entre niveau fondamental et niveau excité permettent d'initialiser le système dans une superposition cohérente pouvant être ensuite manipulée par une deuxième impulsion au cours d'expériences de contrôle cohérent. Le temps de cohérence T2 du système n'est pas seulement limité par la durée de vie radiative T1 et reste très inférieur à la valeur théorique T2= 2T1. Les différents mécanismes de décohérence entrant en jeu ont dès lors été étudiés, en particulier le rôle des phonons acoustiques, responsables d'un fort amortissement des oscillations de Rabi et d'une diminution du temps de cohérence pour une partie des boîtes quantiques étudiées. Nous avons cependant dans certains cas mis en évidence la présence de mécanismes supplémentaires, liés aux fluctuations de l'environnement électrostatique des boîtes. Par ailleurs, une étude poussée de la polarisation de la luminescence émise par ces boîtes, dont la croissance a été réalisée en régime Stranski-Krastanov, a révélé une inclinaison des états propres de la structure fine de l'exciton, ainsi qu'une modification de leur intensité d'émission, témoignant d'un fort mélange des états lourds et légers de la bande de valence
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Modelling the optical properties of semiconducting nanostructuresBuccheri, Alexander January 2016 (has links)
In this thesis we describe the development of a real-space implementation of the Bethe-Salpeter equation (BSE) and use it in conjunction with a semi-empirical tight-binding model to investigate the optoelectronic properties of colloidal quantum- confined nanostructures. This novel implementation exploits the limited radial extent and small size of the atomic orbital basis to treat finite systems containing up to ∼4000 atoms in a fully many-body framework. In the first part of this thesis our tight-binding model is initially benchmarked on zincblende CdSe nanocrystals, before subsequently being used to investigate the electronic states of zincblende CdSe nanoplatelets as a function of thickness. The band-edge electronic states are found to show minimal variation for a range of thicknesses and the results of our tight-binding model show good agreement with those predicted using a 14-band k·p model for a nanoplatelet of 4 monolayers (ML) in thickness. Optical absorption spectra were also computed in the independent-particle approximation. While the results of the tight-binding model show good agreement with those of the 14-band k·p model in the low-energy region of the spectrum, agreement with experiment was poor. This reflects the need for a many-body treatment of optical absorption in nanoplatelet systems. In the second part of this thesis we apply our tight-binding plus BSE model to study the excitonic properties of CdSe nanocrystals and nanoplatelets. Simulations performed on CdSe nanocrystals examined an approximation of the BSE equivalent to configuration interaction singles (CIS), and found that both the optical gap and the low-energy spectral features were unaffected by the approximation. A comparison of exciton binding energies with those predicted by CIS demonstrates the sensitivity of results to the exact treatment of dielectric screening and the decision of whether or not to screen exchange. Our model predicts optical gaps that are in strong agreement with average experimental data for all but the smallest diameters, but was not able to reproduce low-energy spectral features that were fully consistent with experiment. This was attributed to the absence of the spin-orbit interaction in the model. Simulations performed on CdSe nanoplatelets investigate the optical gaps and exciton binding energies as a function of thickness. Exciton binding energies were found to reach ∼200 meV for the thinnest system, however, optical gaps were slightly overestimated in comparison to experiment. This is attributed to the reduced lateral dimensions used in our simulations and our bulk treatment of dielectric screening. A two-dimensional treatment of dielectric screening is expected to further increase binding energies. Calculations of the excitonic absorption spectrum reproduce the characteristic spectral features observed in experiment, and show strong agreement with the spectra of nanoplatelets, with thicknesses ranging from 3 ML to 5 ML.
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Anisotropy and spin relaxation in the condensed phaseHandsel, Jennifer January 2016 (has links)
<strong>Chapter 1</strong> introduces the concept of spin, how spins interact, and how the spin state in a radical pair can affect the outcome of a chemical reaction between the unpaired electrons. The computational methodology for simulating such radical pairs is also discussed. <strong>Chapter 2</strong> discusses anisotropy in the singlet recombination yield of a radical pair in a carotenoid-porphyrin-fullerene triad, containing many hyperfine couplings. The singlet yield was calculated as a function of the direction of an applied magnetic field, using symmetry in the molecule to reduce the size of the problem. The symmetry reduction was partially successful, however it was not possible to include all the hyperfine couplings in the molecule. <strong>Chapter 3</strong> introduces a radical pair located on a flavin ligand and a tryptophan residue in the protein cryptochrome, and discusses the spin-relaxation mechanism of singlet-triplet dephasing. Magnetic field effect curves, describing the formation of a secondary radical pair as a function of applied magnetic field, were found to be broader in longer-lived radical pairs, due to dephasing caused by spin-selective recombination to the singlet ground state. Additional singlet-triplet dephasing may occur due to hopping of one of the unpaired electrons, between a zone of strong exchange interaction and a zone of negligible exchange interaction, although this is an incomplete description of the spin-relaxation. <strong>Chapter 4</strong> discusses the effect of rotational tumbling on spin-relaxation in the flavin-tryptophan radical pair in cryptochrome. Simulations indicated that the resulting modulation of anisotropic hyperfine couplings contributed modestly to spinrelaxation during transient absorption measurements, but was insufficient to explain the lack of an experimental low-field effect, or to explain the width of the experimental magnetic field effect curves as a function of magnetic field strength. <strong>Chapter 5</strong> discusses magnetic field effects on the mutual annihilation of a pair of triplet excitons in tetracene and anthracene crystals. The experimental singlet recombination yield was found, for the first time, to be modulated as a function of the direction of a applied magnetic field as weak as 2 mT. Simulations indicated that this anisotropy arose due to the zero field splitting of the electronic state in each triplet exciton. The direction of the external magnetic field altered the singlet component of the eigenstates of the Hamiltonian, and therefore altered the timeaverage of the singlet probability of a triplet exciton pair. This is different to the already established mechanism under a strong magnetic field, where the anisotropy arises from level crossings of eigenstates.
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Application of quantum Monte Carlo methods to homogeneous electron and electron-hole systemsSpink, Graham George January 2017 (has links)
The properties of the macroscopic world around us, and of which we are a part, are largely determined by the low energy, collective behaviour of many interacting particles, including the nuclei and, especially, the electrons present. Although the fundamental laws governing the behaviour of these many-body systems are believed to be known in principle, the practical solution of the equations of quantum mechanics remains a challenging area of research. This thesis is concerned with the application of quantum Monte Carlo methods to two model systems: the spin-polarised homogeneous electron gas, and a hole-doped electron gas. Electronic structure theory is briefly reviewed before discussing in more detail the quantum Monte Carlo methods used in this thesis. A study of the three-dimensional spin-polarised homogeneous electron gas (HEG) is then reported, where the relatively new technique of twist averaging is investigated in detail and accurate energies and pair correlation functions are obtained over densities $r_s = 0.5 – 20$ a.u. and the full range of spin-polarisation, allowing comparison with the Perdew-Zunger interpolation scheme used in local spin density approximation exchange-correlation functionals. Following this, an impurity is added to the electron gas in the form of a positively charged hole, and the interaction is studied. Relaxation energies, pair correlation functions and momentum densities are reported. Trion formation is observed over a range of carrier densities and electron-hole mass ratios in agreement with experiment. Isolated trions are also studied, where the diffusion Monte Carlo method is exact. Methodological innovations developed while carrying out this work are discussed, including a variance reduction technique for twist-averaged calculations and a new trial wave function for impurity-in-HEG calculations.
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Dinâmica de éxcitons e transporte de cargas em heteroestruturas orgânicas / Exciton dynamics and charge transport in organic heterostructureGustavo Targino Valente 07 December 2017 (has links)
A proposta desse estudo é investigar as propriedades de migração do éxciton, transferência de energia e transporte de cargas em heteroestruturas orgânicas ultrafinas compostas pela integração de um polímero semicondutor com moléculas de clorofila. A sintonização dos estados eletrônicos desses materiais torna possível a obtenção de heteroestruturas com modulação energética capazes de aprisionar éxcitons e cargas apresentando potencialidade de aplicação em Diodos Orgânicos Emissores de Luz (OLEDs). Para tal filmes de polifuoreno (PFO) (camada transportadora de carga) totalmente amorfo e filmes de clorofila (camada ativa na forma de poço de potencial) foram preparados utilizando a técnica e automontagem (LBL) combinada com spin-coating, caracterizados por microscopia confocal por varredura a laser e técnicas espectroscópicas de absorção e emissão. Investigou-se os processos fotofísicos utilizando microscopia confocal e de tempo de vida. Os resultados foram interpretados com base no modelo de transferência de energia de Förster combinado com as taxas de Miller-Abrahams e com a equação de difusão excitônica. Com essa abordagem, obteve-se uma relação entre a migração do éxciton no PFO e a transferência de energia não radiativa deste polímero para as moléculas de clorofila. Observou-se uma eficiente transferência de energia igual a 94% no regime de filmes ultrafinos. Para compreender os mecanismos de transporte de carga, implementamos e validamos o método de simulação de Monte Carlo para o transporte de carga em sistemas orgânicos desordenados. Com essa abordagem investigou-se a dinâmica das cargas em filmes poliméricos desordenados com e sem a camada de poço de potencial. Propriedades elétricas, tais como, mobilidade elétrica e coeficiente de difusão, foram obtidas e estão de acordo com os reportados na literatura. Obteve-se uma taxa de preenchimento de cargas no poço de potencial igual a 1010 buracos/s para campo elétrico de 1 MV/cm e constatou-se que a taxa aumenta com o campo elétrico. Tal abordagem apresenta-se como uma alternativa interessante para auxiliar o planejamento experimental de OLEDs baseados em heteroestruturas orgânicas. / In this study the exciton migration, energy transfer and charge transport in ultrathin organic heterostructure formed by semiconductor polymer and chlorophyll molecules were investigated. The energetic tuning between these materials promotes organic heterostructures with energetic modulation capable of trapping excitons and charges showing an application potential in Organic Light Emitting Diodes (OLEDS). Amorphous polyfluorenes (PFO) and chlorophyll a (chla) were prepared using self-assembly combined with spin-coating methods and characterized by confocal laser scanning microscopy and spectroscopic techniques. Photophysical processes were investigated using confocal and life-time microscopy and the results interpreted from the model of Förster energy combined with the Miller-Abrahams rate as well as the exciton diffusion equation. These results provided a relationship between the exciton migration in the PFO film and the non-radiative energy transfer from polymer to chla molecules. An efficient transfer of energy equal to 94% was observed. Method of the Monte Carlo simulation were implemented to investigate the charge transport in this disordered organic system. Using this method, the charge dynamics with and no potential well layer was studied. Electrical properties obtained, such as electric mobility and diffusion coefficient, are in agreement with literature. It was estimated a charge fill rate in the potential well equal to 1010 holes/s for 1 MV/cm and this parameter increases with the electric field. This approach has been shown to be an interesting alternative for the experimental design of OLEDs composed by organic heterostructure.
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Ressonância magnética detectada eletricamente em diodos de Alq3 / Electrically detected magnetic resonance of Alq3 based diodesGeorge Barbosa da Silva 02 September 2004 (has links)
Ressonância magnética detectada eletricamente (RMDE) de banda-X (9 GHz) e de banda-K (24 GHz) foram usadas para estudar diversos diodos baseados em tris-8(hidroxiquinolinolato) de alumínio III (Alq3). A técnica de RMDE consiste, basicamente, em medir a variação da condutividade quando o sistema entra na condição de ressonância magnética; assim, é possível relacionar propriedades de transporte elétrico com as funções de onda das moléculas envolvidas no processo. Para este estudo foram confeccionados diodos eletroluminescentes e unipolares de multicamadas no Laboratoire d'Optoélectronique des Materiaux Moléculaire (LOMM), da École Polytechnique Fédérale de Lausane (EPFL), Suíça, pelo Dr. Frank Nüesch. Faz parte também deste trabalho a montagem experimental do sistema de RMDE de banda-K, onde a maior parte dos dados foram obtidos. O sinal de RMDE dos diodos unipolares, da ordem de 1E-6, é atribuído ao processo dependente de spin de saltos eletrônicos que ocorre próximo às interfaces. O sinal típico de RMDE dos diodos eletroluminescentes é mais intenso, da ordem de 1E-4, e é atribuído à ressonância de spin-1/2 na formação dos éxcitons. O espectro de RMDE, por meio de ajuste de curvas, pôde ser decomposto em duas gaussianas: uma com largura de linha pico-a-pico DHPP de 1,6 mT, independente do campo elétrico aplicado no dispositivo, e outra variando de 2,0 mT a 3,4 mT. A componente mais estreita se deve à ressonância do radical positivo de Alq3, enquanto que a componente mais larga àquela do negativo. O estudo da forma de linha e de sua dependência com o campo elétrico dos espectros de RMDE de diodos unipolares dão suporte à ambas as atribuições. Neste trabalho, a questão da eficiência quântica e da zona de recombinação também são discutidas. / Electrically Detected Magnetic Resonance (EDMR) at X-band (9GHz) and K-band (24 GHz) were used to investigate Alq3 based diodes. EDMR technique consists basically of measuring conductivity variation at magnetic resonance conditions; thus, it is possible to correlate electrical transport properties with wave functions of the molecules involved in the process. Electroluminescent and unipolar multilayer diodes were prepared in the Laboratoire d'Optoélectronique des Materiaux Moléculaire (LOMM), at on École Polytechnique Fédérale de Lausane EPFL, Switzerland by Dr. Frank Nüesch. The experimental setup of the K-band EDMR system, where most of the data were obtained, was also part of this work. The unipolar diodes EDMR signal is of the order of 1E-6 and is attributed to spin dependent hopping process close to the interfaces. The electroluminescent diodes typical EDMR signal is more intense, of the order of 1E-4 , and is attributed to exciton´s formation spin-1/2 resonance. The EDMR spectrum can be decomposed into two Gaussians: one with peak-to-peak line width (DHPP) of 1.6 mT, independent of the electrical field applied to the devices, and other one whit DHPP of 2.0 mT to 3.4 mT. The narrower component is due to the resonance of positive Alq3 radical, while the larger component is due to the negative. Both attributions are supported by the investigation of line shape and its dependence of electrical field in the unipolar diodes EDMR spectra. In this work, the quantum efficiency and the recombination zone issues are also discussed.
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Propriétés des boites quantiques GaAs/AlGaAs obtenues par remplissage des nanotrous / Properties of GaAs/AlGaAs quantum dots obtained by nanohole infillingPankratov, Andrey 14 March 2017 (has links)
Le but de cette thèse a été de caractériser des boîtes quantiques obtenues avec une nouvelle méthode de croissance. Utilisant des techniques de microphotoluminescence, nous avons étudié les différentes contributions au mélange des bandes de trous lourds et de trous légers. En l'absence de contrainte, la distribution du paramètre de mélange est plus homogène ; cependant, d'autres contributions deviennent dominantes et nous les avons discutées. Nous avons mesuré les paramètres magnéto-optiques : facteurs Landé de l'électron et du trou, décalage diamagnétique, paramètres de structure fine des états noirs et brillants. Les valeurs obtenues ont permis d'estimer la variation des paramètres géométriques des boîtes, ce qui est lié à la qualité du contrôle de la croissance. La polarisation des états noirs mesurée s'est révélée différente de celle prévue selon le modèle utilisé précédemment dans la littérature. Utilisant un modèle théorique récent, nous avons reproduit nos observations, ce qui met en évidence une modulation possible de la polarisation des états noirs par le champ magnétique. Finalement, nous avons effectué des études de contrôle de charges dans des structures n-i Schottky. Pour des boîtes uniques, des états multichargés ont été observés. Nous avons mesuré les énergies de liaison des trions positif et négatif, au préalable à une étude sur des molécules de boîtes. Nous avons observé des anticroisements des états S des trous dans deux boîtes, en accord avec nos prévisions basées sur les paramètres nominaux de l'échantillon. / The goal of this thesis work was to characterise quantum dots obtained by a novel growth method. We used microphotoluminescence techniques to study multiple properties of these dots. We have evaluated main contributions to light-heavy hole valence band mixing. Contrary to self-assembled dots, we find a more homogeneous distribution of the mixing parameter, which can be explained by the absence of mechanical tension due to lattice mismatch. We have also measured magneto-optical parameters such as electron and hole g-factors, diamagnetic shift, fine structure splitting for bright and dark states. These results allowed us to estimate geometric parameters of dots, making a point on the growth quality. Polarisation studies on the dark states have revealed a result different from previous theoretical predictions. We have used a recently presented model to explain our findings. The last part of this work presents results on quantum dots embedded in an n-i Schottky structure. We have measured binding energies of positive and negative trions, to make a connection with previous results, to then study double quantum dot system. We have observed an anticrossing of hole S states, which is in agreement with our estimations based on sample parameters.
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Deep ultraviolet photoluminescence studies of Al-rich AlGaN and AlN epilayers and nanostructuresNepal, Neeraj January 1900 (has links)
Doctor of Philosophy / Department of Physics / Hongxing Jiang / Deep ultraviolet (UV) photoluminescence (PL) spectroscopy has been employed to study optical properties of AlGaN alloys, undoped and doped AlN epilayers and nanostructure AlN photonics crystals (PCs). Using a deep UV laser system with an excitation wave length at 197 nm, continuous wave PL, temperature dependent, and time-resolved PL have been carried out on these AlGaN and AlN epilayers and nanostructures.
We have measured the compositional and temperature dependence of the energy bandgap of AlxGa1-xN alloys covering the entire alloy range of x, 0 ⤠x ⤠1 and fitted with the Varshni equation. Varshni coefficients, alpha and betaï¬ in AlGaN alloys have a parabolic dependence with alloy concentration x. Based on the experimental data, an empirical relation was thus obtained for the energy gap of AlGaN alloys for the entire alloy concentration and at any temperature below 800 K.
The exciton localization energy in AlxGa1-xN alloys the entire composition range (0 ⤠x ⤠1) has been measured by fitting the band edge emission peak energy with the Varshni equation. Deviations of the excitonic emission peak energy from the Varshni equation at low temperatures provide directly the exciton localization energies, ELoc in AlGaN alloys. It was found that ELoc increases with x for x ⤠0.7, and decreases with x for x ⥠0.8. The relations between the exciton localization energy, the activation energy, and the emission linewidth have been established. It thus provides three different and independent methods to determine the exciton localization energies in AlGaN alloys.
Impurity transitions in AlGaN alloys have also been investigated. Continuous wave (CW) PL spectra of Si and undoped AlGaN alloys reveals groups of impurity transitions that have been assigned to the recombination between shallow donors and an isolated triply charged cation-vacancy (VIII)3-, a doubly charged cation-vacancy-complex (VIII-complex)2-, and a singly charged cation-vacancy-complex (VIII-complex)-1. The energy levels of these deep acceptors in AlxGa1-xN (0 ⤠x ⤠1) alloys are pinned to a common energy level in the vacuum. AlGaN alloys predominantly exhibiting the bandedge and (VIII-complex)1- transitions possess improved conductivities over those emitting predominantly (VIII)3- and (VIII-complex)2- related transitions. These results thus answer the very basic question of high resistivity in Al-rich AlGaN alloys.
Acceptor doped AlGaN alloys have been studied by deep UV PL. A PL emission line at 6.02 eV has been observed at 10 K in Mg-doped AlN. It is due to the recombination of an exciton bound to the neutral Mg acceptor (I1) with a binding energy, Ebx of 40 meV, which indicates large activation energy of the Mg acceptor. The observed large binding energy of the acceptor-bound exciton is consistent with relatively large binding energy of the Mg acceptor in AlN.
With the energy level of 0.51 eV for Mg dopants in AlN, it is interesting and important to study other suitable acceptor dopants for AlN. Growth and optical studies of Zn-doped AlN epilayers has been carried out. The PL spectra of Zn-doped AlN epilayers exhibited two impurity emission lines at 5.40 and 4.50 eV, which were absent in undoped epilayers. They are assigned respectively, to the transitions of free electrons and electrons bound to triply positively charged nitrogen vacancies (0.90 eV deep) to the Zn0 acceptors. It was deduced that the Zn energy level is about 0.74 eV above the valence band edge, which is about 0.23 eV deeper than the Mg energy level in AlN.
Nitrogen vacancies are the compensating defects in acceptor doped AlGaN alloys. A nitrogen vacancy (VN) related emission line was also observed in ion-implanted AlN at 5.87 eV and the energy level of singly charged VN1+ is found at 260 meV below the conduction band. As a consequence of large binding energy of VN1+ as well as high formation energy, VN1+ in AlN cannot contribute significant n-type conductivity, which is consistent with experimental observation.
The temperature dependent PL study of the bandedge emissions in GaN and AlN epilayers up to 800 K has been carried out, which reveals two distinctive activation processes. The first process occurring below Tt = 325 K (Tt = 500 K) for GaN (AlN) is due to the activation of free excitons to free carriers, whereas the second occurring above Tt with an activation energy of 0.29 eV (0.3 eV) for GaN (AlN) is believed to be associated with a higher lying conduction band (ï3) at about 0.3 eV above the conduction band minimum (ï1). These higher lying bands could affect device performance of GaN and AlN at elevated temperatures.
Two-dimensional nanostructured AlN photonic crystals (PCs) with a varying periodicity/diameter down to 150 nm/75 nm have also been studied by deep UV PL. With PCs formation, a 20-fold enhancement in the band edge emission intensity at 208 nm over unpatterned AlN epilayer has been observed. The emission intensity increases with the decrease in the lattice constant of the AlN PCs. AlN PCs represent photonic crystals with highest (shortest) bandgap (wavelength) semiconductors, which open up new opportunities for exploring novel physical phenomena in the artificially structured photonic band gap material systems and their applications, particularly in the area of deep UV as well as nano-photonics.
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