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Excitações coletivas em sistemas eletrônicos quasi-2d via espalhamento inelástico de luzGonçalves, Alison Arantes 08 March 2012 (has links)
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Previous issue date: 2012-03-08 / CAPES - Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / Apresentamos uma teoria para obtenção da seção de choque de espalhamento inelástico de luz, espalhamento Raman, a temperatura de T = OK em um gás de elétrons quasi-bidimensional formado pela heteroestrutura semicondutora de A1GaAs-GaAs dopada seletivamente. Os cálculos de estrutura eletrônica foram baseados na Teoria do Funcional Densidade dentro da aproximação de densidade local. Os cálculos para a seção de choque foram realizados em geometria de retroespalhamento e em regime de ressonância do laser incidente com o gap ótico de spin-órbita do GaAs. Estudamos os mecanismos de excitações de densidade de carga e excitações de densidade de spin. Os resultados obtidos foram [1]: 1) a observação do colapso do termo de Hartree nas excitações de densidade de carga para baixas densidades, observado experimentalmente por Ernst et al. [2]; 2) a observação de um cruzamento anômalo entre as excitações de densidade de carga e densidade de spin, em virtude dos funcionais de exchange-correlação. Este efeito constitui um teste de validade para as parametrizações adotadas; 3) a predição da existência de excitações de mais alta energia, ainda não observadas experimentalmente. Finalmente, demonstramos que o formalismo desenvolvido permite mapear as excitações eletrônicas na teoria BCS. / We present a theory for obtaining the inelastic light scattering cross section, Raman scattering, at T = OK temperature in a quasi-bidimensional electron gas formed by the GaAs-A1GaAs semiconductor heterostructure doped selectively. The electronic structure calculations were based on Density Functional Theory within the local density approximation. The calculations for the cross section were performed in backscattering geometry and resonant regime of the incident laser with the spin-orbit optical gap of GaAs . We study charge density excitations mechanism and spin density excitations mechanism. Our results were as follows [1] 1) the observation of the collapse of the Hartree term in the charge density excitation for low densities, observed experimentally by Ernst et al. [2], 2) the observation of an anomalous cross between charge density and spin density excitations, due to the exchange-correlation functional. This effect is a validity test for the adopted parameterizations; 3) the prediction of the existence of excitations of higher energy, not yet observed experimentally. Finally, we demonstrate that the formalism developed enables mapping the electronic excitations in the BCS theory, which describes the normal superconducting state.
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Electrical and optical characterization of beta-Ga2O3Fiedler, Andreas 03 January 2020 (has links)
Diese Arbeit beschäftigt sich mit der Bewertung des Breitband-Halbleiters ß-Ga2O3 für die Hochleistungselektronik. Daher sind Schichten, die mit metallorganischer Gasphasenepitaxie (MOVPE) gewachsen sind, und Volumenkristalle, die mit der Czochralski-Methode gewachsen sind, elektrisch und optisch charakterisiert. Dabei werden die grundlegenden Eigenschaften des Materials untersucht und mit den theoretischen Vorhersagen verglichen. Der Einfluss und die Bildung von Defekten werden untersucht.
Zu Beginn zeigten die MOVPE-gewachsenen Schichten ungünstige elektrische Eigenschaften, da sie bei niedrigeren Dotierungskonzentrationen vollständig kompensiert wurden und bei höheren Ladungsträgerkonzentrationen eine geringere Ladungsträgerbeweglichkeit aufwiesen. Ein quantitatives Modell des schädlichen Einflusses inkohärenter Zwillingsgrenzen auf elektrische Eigenschaften wird entwickelt, das zeigt, dass die Verhinderung der Bildung von diesen der Schlüssel zur Verbesserung des Materials ist. Die Dichte der inkohärenten Zwillingsgrenzen wurde um 4 Größenordnungen reduziert, was zu einer verbesserten Ladungsträgerbeweglichkeit führte. Dies bietet eine vielversprechende Perspektive für den Einsatz von ß-Ga2O3 in zukünftiger Leistungselektronik.
Ramanspektroskopische Untersuchungen an hoch n-dotierten Kristallen zeigen die Bildung eines Störstellenbandes, geben Einblicke in die effektivmasseartige Donatornatur von Si und Sn und zeigen zusätzliche Raman-verbotene, longitudinale Phononen-Plasmonmoden durch Streuung durch Fluktuationen der freien Ladungsträgerdichte.
Die relative statische Dielektrizitätskonstante von ß-Ga2O3 senkrecht zu den Ebenen (100), (010) und (001) wird auf 10,2, 10,87 bzw. 12,4 bestimmt, die eine zuverlässige Grundlage für die Simulation und Konstruktion von Bauelementen bilden.
Die Erzeugung von heller, roter Elektrolumineszenz (EL) in Sperrrichtung betriebenen Schottky-Barrieredioden auf der Basis von mit Cr und Si co-dotierten Kristallen wird gezeigt. Die EL von Cr ist repräsentativ für die Fähigkeit, die lumineszierenden Zustände anderer Übergangsmetalle anzuregen. Solche lichtemittierenden Schottky-Barrieredioden können ein neues Anwendungsgebiet von ß-Ga2O3 eröffnen. / This thesis deals with the evaluation of the wide band gap semiconductor ß-Ga2O3 for high power electronics. Therefore, layers grown with metal-organic vapor phase epitaxy (MOVPE) and bulk crystals grown by Czochralski method are electrically and optically characterized. Hereby, the fundamental properties of the material are investigated and compared with the theoretical predictions. The influence and formation of defects are investigated.
At the beginning the MOVPE grown layers showed unfavorable electrical properties as they were fully compensated at lower doping concentrations and showed lowered mobility at higher charge carrier concentrations. A quantitative model of the detrimental influence of incoherent twin boundaries on electrical properties is developed showing that the prevention of the formation of these is the key to improve the material. The density of incoherent twin boundaries was reduced by 4 orders of magnitude resulting in improved charge carrier mobility. This provides a promising outlook for the use of ß-Ga2O3 in future power electronics.
Raman spectroscopic investigations of highly n-type doped crystals reveal the formation of an impurity band, give insight in the effective-mass like donor nature of Si and Sn, and show additional Raman forbidden, longitudinal phonon plasmon modes due to free-electronic-charge density fluctuations scattering.
The relative static dielectric constant of ß-Ga2O3 perpendicular to the planes (100), (010), and (001) is determined to 10.2, 10.87, and 12.4, respectively, which give a reliable basis for the simulation and design of devices.
The generation of bright, red electroluminescence (EL) in reverse biased Schottky barrier diodes based on crystals co-doped with Cr and Si is shown. The EL of Cr is representative of the ability to excite the luminescent states of other transition metals. Such light emitting Schottky barrier diodes may open up a new application field of ß-Ga2O3.
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Investigation of device related material properties of β-Ga2O3 bulk crystals and homoepitaxial layersSeyidov, Palvan 14 February 2024 (has links)
Die zentrale wissenschaftliche Fragestellung dieser Arbeit ist die Bewertung von anwendungsorientierten (100) β-Ga2O3 Czochralski (Cz) gewachsenen Bulk-Kristallen und mit metallorganischer Gasphasenepitaxie (MOVPE) gewachsenen homoepitaktischen Schichten. Zur Charakterisierung der Kristalle wurden elektrische und optische Charakterisierungsmethoden angewandt. Die Ergebnisse der Untersuchungen lassen sich wie folgt zusammenfassen: Das Wachstum der Bulk-Kristalle erfolgt bevorzugt nach der Cz-Methode bei Temperaturen um 1800°C. Bei einer so hohen Temperatur ist der unbeabsichtigte Einbau von Verunreinigungen in den Kristall unvermeidlich, insbesondere von dem Übergangsmetall Iridium (Ir) aus den Ir-Tiegeln. In diesem Zusammenhang wurde resonante elektronischer Raman-Streuung (ERS) untersucht, die von Ir4+-Ionen in β-Ga2O3 aus der Cz-Züchtung stammt. Der beobachtete ERS-Peak bei 5150 cm-1 wird einem internen Übergang innerhalb des gespaltenen 2T2g-Grundzustands der Ir4+-Ionen zugeschrieben. Die optischen und elektrischen Eigenschaften von 3d-TM Co und Ni in β-Ga2O3 wurden experimentell und theoretisch untersucht. Optische Absorptionsspektroskopie, Messungen der Photoleitfähigkeit und Berechnungen der Ladungszustandsübergangsniveaus auf der Grundlage der Dichtefunktionaltheorie wurden kombiniert. Ein (+/0)-Donor-Niveau ~ 0,7 eV, ~ 1,3 eV oberhalb des Valenzband-Maximums und ein (0/-)-Akzeptor-Niveau ~ 2 eV, ~ 2,8 eV unterhalb des Leitungsband-Minimums wurden konsistent für Co- bzw. Ni-dotierte Kristalle abgeleitet. Aufgrund der mittleren Bandlückenposition des Akzeptorniveaus und des daraus resultierenden höheren extrapolierten Widerstandes bei Raumtemperatur schlagen wir vor, dass Co und Ni geeignete Kandidaten für die Kompensationsdotierung von halbisolierenden β-Ga2O3-Bulkkristallen sind. / The core scientific question of this thesis is the evaluation of device-related (100) β-Ga2O3 Czochralski (Cz) grown bulk crystals and metal-organic vapor phase epitaxy (MOVPE)-grown homoepitaxial layers. Electrical and optical characterization methods were applied to characterize the crystals. The findings of the investigations can be summarized as follows: The growth of the bulk crystals is preferentially performed by the Cz method at temperatures around 1800°C. At such a high temperature, the unintentional incorporation of impurities into the crystal is inevitable, especially transition metal iridium (Ir) from the Ir crucibles. In this respect, the observation of resonant electronic Raman scattering (ERS) originating from Ir4+ ions in bulk β-Ga2O3 grown by the Cz method was studied. The observed ERS peak at 5150 cm-1 is attributed to an internal transition within the split 2T2g ground state of Ir4+ ions. The optical and electrical properties of the 3d-TM Co and Ni in bulk β-Ga2O3 were experimentally and theoretically investigated. Optical absorption spectroscopy, photoconductivity measurements, and charge-state transition-level calculations based on density functional theory were combined. A (+/0) donor level ~ 0.7 eV, ~ 1.3 eV above the valence band maximum, and a (0/–) acceptor level ~ 2 eV, ~ 2.8 eV below the conduction band minimum are consistently derived for Co- and Ni- doped crystals, respectively. Based on the mid-band gap position of the acceptor level and the resulting higher extrapolated resistivity at room temperature, we propose Co and Ni are suitable candidates for compensation doping of semi-insulating β-Ga2O3 bulk crystal.
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Sensing Interfacial Non-Faradaic and Faradaic Processes via Plasmonic-Enhanced Metallic Luminescence in Nano-OptoelectrodesZhao, Yuming 03 January 2024 (has links)
Metallic nanostructures supporting surface plasmon modes can concentrate optical fields, and enhance luminescence processes from the metal surface at plasmonic hotspots. Such nanoplasmonic metal luminescence contributes to the spectral background in surface-enhanced Raman spectroscopy (SERS) measurements and is helpful in bioimaging, nano-thermometry, and chemical reaction monitoring applications. Despite increasing interest in nanoplasmonic metal luminescence, little attention has been paid to investigating its dependence on voltage modulation. Also, the hyphenated electrochemical surface-enhanced Raman spectroscopy (EC-SERS) technique typically ignores voltage-dependent spectral background information associated with nanoplasmonic metal luminescence due to limited mechanistic understanding and poor measurement reproducibility. In this thesis, we combine the experimental observations and theoretical study on dynamic Faradaic & non-Faradaic modulated nanoplasmonic metallic luminescence and molecular vibrational Raman from hotspots at the electrode-electrolyte interfaces using multiple novel nano-optoelectrodes. Our work represents a critical step toward the general application of nanoplasmonic metal luminescence signals in optical voltage biosensing, hybrid optical-electrical signal transduction, and interfacial electrochemical monitoring. / Master of Science / Understanding the non-Faradaic and Faradaic process pathway is crucial for unraveling reaction mechanisms, developing efficient catalysts, designing bionsensing methodology, energy conversion and cellular stimulator (1-7). Advances in spectroscopic techniques( 8, 9) and computational models (3, 10) have facilitated the investigation of the non-Faradic and Faradaic processes. Unlike bulk reactions, interfacial electrochemical reactions occur in nanometer-thin layers (3, 11), necessitating highly sensitive detection methods. A significant challenge is background interference from bulk electrolytes and electrodes, often obscuring weak signals from the interfacial region – traditional spectroelectrochemistry struggles to match the high temporal resolution requirement due to noise (12, 13). Surface plasmons have become a promising solution for enhancing the sensitivity of spectroelectrochemical techniques (14, 15). Surface plasmons are collective oscillations of electrons at the metal-dielectric interface, which can focus and intensify optical fields at the nanoscale (16), boosting diverse nonlinear emission signals, including fluorescence, Raman scattering, and harmonic generation (17-23). By utilizing surface plasmons, spectroelectrochemistry techniques have shown promise in detecting interfacial activities with high sensitivity. In this thesis, we introduce a pioneering dual-channel in situ EC-SERS methodology, which harnesses the synergy between plasmon-enhanced vibrational Raman scattering (PE-VRS) and plasmon-enhanced electronic Raman scattering (PE-ERS) interfacial signals to monitor and analyze the Faradaic and non-Faradaic process at the electrode-electrolyte interfaces.
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Sobre a natureza das excitações de partícula independente em gás de elétrons bidimensional via espectroscopia Raman ressonanteRodrigues, Leonarde do Nascimento 16 September 2016 (has links)
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Previous issue date: 2016-09-16 / CAPES - Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / O espalhamento inelástico de luz tem sido extensivamente utilizado no estudo de materiais semicondutores e se tornou uma técnica indispensável para o entendimento de processos físicos fundamentais. Os efeitos das interações em sistemas eletrônicos quantizados como o gás de elétrons bidimensional foram investigados por meio do espalhamento inelástico de luz, o qual permite entender a natureza das excitações coletivas que são conhecidas como excitações de densidade de carga (CDE) e excitações de densidade de spin (SDE). CDE são oscilações plasmônicas resultantes do acoplamento entre as flutuações de carga via interações de Coulomb e correlação e troca, enquanto SDE ocorrem apenas em decorrência da presença dos efeitos de correlação e troca. CDE são ativas quando a energia do laser é ressonante com o gap óptico do semicondutor (regime de ressonância próxima) e as polarizações da luz incidente e espalhada são paralelas entre si. SDE é também ativa em condições de ressonância próxima e possui polarizações da luz incidente e espalhada perpendiculares entre si. Todavia, tal cenário rompe quando a luz do laser coincide com as energia das transições interbandas do material (regime de ressonância extrema). Em adição as excitações coletivas emergem transições anômalas de gás de elétrons tipo não interagente conhecidas como excitações de partícula independente (SPE). A física envolvida em tais transições ainda parece não ser completamente entendida. Neste trabalho, são apresentados resultados experimentais e teóricos via espalhamento Raman eletrônico oriundos de gás de elétrons bidimensional realizados a partir de poços quânticos simples com o intuito de compreender a natureza das excitações de partícula independente. A medida experimental e os cálculos presentes na tese consistem de um poço quântico simples de 250Å de GaAs (arseneto de gálio) com dopagem modular e densidade eletrônica total de 8.81 x 1011cm-2. Também foi considerado o acoplamento das flutuações de densidade de carga com o fônon óptico longitudinal do GaAs. Em adição, é realizado um cálculo teórico de uma estrutura de poço quântico simples considerado estreito de 100Å de GaAs com dopagem modular e densidade eletrônica total de 1.2 x 1012cm-2. Portanto, o objetivo deste trabalho é mostrar em um caminho claro e transparente a situação física da existência das excitações eletrônicas em gás de elétrons. O trabalho mostrou que, no regime de extrema ressonância, as oscilações de plasma se dividem em duas contribuições: um conjunto de excitações coletivas renormalizadas (plasmons) e transições eletrônicas não renormalizadas (SPE). A fim de alcançar esse propósito, o trabalho evidenciou que o espalhamento Raman eletrônico pertence a uma mesma classe de problemas como o oscilador harmônico amortecido, acoplado e forçado assim como o estado supercondutor na teoria BCS de metais normais. A comparação entre os dados experimentais e teóricos mostrou um excelente acordo. / The inelastic light scattering has been widely used in the study of the semiconductor materials and it has become an indispensable technique for the understanding of fundamental physical processes. The effects of the electronic interactions on quantized electronic systems as two-dimensional electron gas are investigated through means of Raman scattering which allows understand the nature of collective excitations which are known as charge density excitations (CDE) and spin density excitations (SDE). CDE are plasmonic oscillations arising from the coupling between charge fluctuations via Coulombian and exchange-correlation interactions while SDE occur only when exchange-correlation effects are present. CDE is active when the laser energy is resonant with a semiconductor optical gap (near resonance regime) and the incoming and outgoing light polarizations are parallel to each other and SDE has incoming and outgoing light polarizations perpendicular to each other. Nevertheless, such a picture breaks down when the laser matches interband transitions energies of the material (extreme resonance regime). In addition to the collective excitations emerge anomalous transitions of the electron gas noninteracting-like known as single-particle excitations (SPE). The physics of such transitions is still not completely understood. In this work, were present experimental and theoretical results via electronic Raman scattering originating from the two-dimensional electron gas carried out from single quantum wells with the aim of understand the nature of the single-particle excitations. The experimental measures and calculations present in the thesis consists of the GaAs (gallium arsenide) single quantum well of a 250Å wide with modulation-doped and total electronic density of 8.81 x 1011cm2. It was also considered the coupling of the charge fluctuations with the longitudinal optical phonon of GaAs. In addition, it is performed a theoretical calculation of a structure of the GaAs single quantum well considered narrow of a 100Å wide with modulation-doped and and total electronic density of 1.2 x 1012cm2. However, the goal of this work is to show in a clear and transparent way the physical situation of the existence of electronic excitaions in electron gas. The work showed that, in extreme resonance regime, the plasma oscillations splits into two contributions: a set of renormalized collective excitations (plasmons) and unrenormalized electronic transitions (SPE). In order to accomplish this purpose, the study showed that electronic Raman scattering belongs to the same class of problems such as a set of forced, coupled and damped harmonic oscillators or formation of the superconducting state in BCS theory of normal metals. Comparison between experiment and theory shows an excellent agreement.
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