Neste trabalho estudamos propriedades termodinÃmicas de um gÃs de elÃtrons confinado em uma superfÃcie bidimensional cilÃndrica sob a aÃÃo de um campo magnÃtico perpendicular ao eixo do cilindro. Observamos que o campo magnÃtico aplicado desta forma produz efeito similar ao produzido por um campo magnÃtico nÃo-homogÃneo em um sistema plano. Calculamos o espectro de energia nesse sistema para diferentes valores de curvatura e simetria do campo com a superfÃcie. Mostramos que as propriedades fÃsicas desses sistemas estÃo fortemente ligadas a essa simetria do campo magnÃtico atravÃs do cÃlculo da densidade de estados, potencial quÃmico e calor especÃfico do sistema. Investigamos como a curvatura de um filme semicondutor afeta suas propriedades eletrÃnicas e de transporte. Estudamos como o potencial efetivo induzido pelas deformaÃÃes de curvatura periÃdicas no filme modificam sua estrutura de bandas induzindo o confinamento eletrÃnico. Para parÃmetros fixos de curvatura, tal confinamento pode ser ajustado atravÃs de um campo elÃtrico externo, de modo que certas caracterÃsticas da estrutura de bandas tais como emph{gaps} de energia e curvaturas das bandas podem ser controladas por um parÃmetro externo. TambÃm mostramos que, para alguns valores de curvatura e campo elÃtrico, Ã possÃvel obter bandas de Dirac para filmes semicondutores com curvatura Gaussiana. AlÃm disso, usamos um mÃtodo de propagaÃÃo de pacotes de onda para demonstrar que as curvaturas sÃo responsÃveis por significantes transiÃÃes entre sub-bandas, especialmente para valores moderados de curvatura. / We study thermodynamic properties of an electron gas confined in a two-dimensional cylindrical surface under the action of a magnetic field perpendicular to the cylinder axis. We observed that the applied magnetic field has a similar effect to that produced by a non-homogeneous magnetic field on a flat system. We calculate the energy spectrum of the system for different values of curvature and symmetry of the magnetic field to the surface. We show that the physical properties of these systems are strongly connected to the symmetry imposed by the magnetic field by calculating the density of states, specific heat and chemical potential. We investigate how the curvature of a semiconductor film affects its electronic and transport properties. We study how the geometry-induced potential resulting exclusively from periodic ripples in the film modifies its band structure by inducing electronic confinement. For fixed curvature parameters, this confinement can be easily tuned by an external electric field, so that features of the band structure such as the energy gaps and band curvature can be controlled by an external parameter. We also show that, for some values of curvature and electric field, it is possible to obtain massless Dirac bands for a smooth structure. Moreover, we use a wave packet propagation method to demonstrate that the ripples are responsible for a significant inter-sub-band transition, specially for moderate values of the ripple height.

Submitted by Irene Nascimento (irene.kessia@ufpe.br) on 2016-07-12T19:51:09Z No. of bitstreams: 2 license_rdf: 1232 bytes, checksum: 66e71c371cc565284e70f40736c94386 (MD5) Elizane Efigenia de Moraes.pdf: 9079354 bytes, checksum: 7ee5a581c6d0b14cdc6b518cd6aa7276 (MD5) / Made available in DSpace on 2016-07-12T19:51:09Z (GMT). No. of bitstreams: 2 license_rdf: 1232 bytes, checksum: 66e71c371cc565284e70f40736c94386 (MD5) Elizane Efigenia de Moraes.pdf: 9079354 bytes, checksum: 7ee5a581c6d0b14cdc6b518cd6aa7276 (MD5) Previous issue date: 2015-07-30 / Nesta dissertação estudamos as propriedades de transporte do nitreto de boro cúbico (cBN, para a sigla em inglês) com as superfícies de uma amostra de quatro camadas passivadas com hidrogênio: em uma superfície o H se liga ao B e na outra ao N. As características do transporte são investigadas com a introdução de dois eletrodos de ouro (Au), em equilíbrio eletrostático com a amostra e submetidos a uma diferença de potencial V em intervalos de interesse: 0:2 V 0:2, 1 V 1 e 3 V 3. O teste de tunelamento com voltagem nula também foi realizado. As principais propriedades observadas são brevemente relatadas em seguida: (i) Os eletrodos são idênticos (no cálculo inicial do programa Siesta adicionamos uma camada "tampão"de átomos, a qual é desconsiderada no programa Transiesta-propriedades de transporte. A simetria dos eletrodos (esquerda e direita) se manifesta com PDOS idênticos para voltagem nula nos intervalos de energia investigados; (ii) A característica I-V (corrente versus voltagem) da amostra apresenta um pico acentuado para V 0:25. A origem deste pico é atribuída à ocorrência do nível quase localizado do H, situado abaixo do nível de Fermi e hibridizado com estados sp3 do B, como evidenciado no cálculo de DFT (Siesta) da estrutura eletrônica e densidade de estados do sistema de quatro camadas. De fato, uma análise dos PDOS dos eletrodos e da amostra sugere que esta interpretação é compatível com o cálculo numérico do Transiesta para o tunelamento através da amostra e o cálculo das características IV através da Fórmula de Landauer-Büttiker: na configuração de equilíbrio mencionada, as correntes máximas obtidas foram Imax(V = 0:25 Volts ) = 163 pico Ampéres (pA) e Imax(V = 2:5 ) = 380 pA. (iii) Enfatizamos que, no intervalo 0:2 V 0:2 a característica IV é muito semelhante àquela observada em diodos de junção p-n. Por outro lado, no intervalo 3 V 3 a retificação é bem menos efetiva para jV > 0:2j ; (iV) outra observação de destaque é o aumento da corrente, isto é, jImax(V = 0:8 )j = 9:85 nano Ampéres (nA) quando a distância dos eletrodos e a amostra é diminuída. Os resultados sugerem o prosseguimento e o aprofundamento das investigações, tendo em vista o uso potencial do cBN passivado com hidrogênio em dispositivos eletrônicos. / In this thesis we study the transport properties of cubic boron nitride (cBN) with the surfaces of a sample of four layers hydrogen terminated hydrogen: on a surface, H binds to B and on the other, to N. The characteristics of the transport are investigated after the introduction of two gold electrodes in an electrostatic equilibrium with the sample and subjected to a potential difference V in intervals of interest:0:2 V 0:2, 1 V 1 e 3 V 3. Tunneling test with zero voltage was also made. The main observed properties are reported briefly: (i) the electrodes are identical (within a layer buffer atoms only considered in the initial calculation Siesta program, to simulate a bulk behavior, therefore it is not considered in Transiesta program, that is, for the calculation of transport properties). The symmetry of electrodes (left and right) manifests with identical PDOS to zero voltage in between the energy intervals investigated; (ii) The IV characteristic (current versus voltage) of the sample shows a sharp peak for V 0:25. The origin of this peak is attributed to the occurrence of nearly located H level, situated below the Fermi level and hybridized with sp3 states of B, and evidenced in the DFT calculation (Siesta) of the electronic structure and density of states of the four layer system. The PDOS electrode and the sample analyses suggest that this interpretation is compatible with Transiesta numerical calculation of the tunneling through the sample and to calculate the current versus voltage I (V) by the Landauer-Büttiker formula: the aforementioned balance setting, the maximum currents obtained were Imax(V = 0:25 Volts ) = 163 peak amps (pA) and Imax(V = 2:5 ) = 380 pA; (iii) - Another important observation was the increase in current, i.e. jImax(V = 0:8 )j = 9:85 nano amps (nA) when the distance of the electrodes and the sample is reduced. The results suggest the continuation and deepening of the study, considering the potential use of CBN passivated with hydrogen in electronic devices.

Submitted by Fabio Sobreira Campos da Costa (fabio.sobreira@ufpe.br) on 2017-02-15T13:24:58Z No. of bitstreams: 2 license_rdf: 1232 bytes, checksum: 66e71c371cc565284e70f40736c94386 (MD5) Dissertação_Mestrado_FaniaCM.pdf: 2231632 bytes, checksum: bb26fa0342704fd41ad5ba76719deac0 (MD5) / Made available in DSpace on 2017-02-15T13:24:59Z (GMT). No. of bitstreams: 2 license_rdf: 1232 bytes, checksum: 66e71c371cc565284e70f40736c94386 (MD5) Dissertação_Mestrado_FaniaCM.pdf: 2231632 bytes, checksum: bb26fa0342704fd41ad5ba76719deac0 (MD5) Previous issue date: 2015-06-30 / FACEPE / Recentes progressos na fabrica¸c˜ao de nanoestruturas fornecem a possibilidade de produzir filmes finos que contenham defeitos artificiais como s´ıtios de aprisionamento com tamanho, geometria e disposi¸c˜ao espacial bem definidas. O estudo dessa introdu¸c˜ao de um arranjo regulardedefeitosemfilmesfinossupercondutoresdotipoIItemsidoativamentedesenvolvido desde o ponto de vista te´orico e experimental, por um lado pela riqueza de comportamentos est´aticos e dinˆamicos que apresenta e, por outro, pela compreens˜ao dos mecanismos para estabilizareancorararededev´orticescontraasfor¸casmotorasexternas. Umdosfenˆomenos mais not´aveis destes sistemas ´e chamado efeito matching, o qual ocorre quando o n´umero de v´ortices ´e um m´ultiplo inteiro do n´umero dos centros de aprisionamento, sendo observados picos na corrente cr´ıtica (resposta est´atica) ou atenua¸c˜oes na mobilidade dos v´ortices (resposta dinˆamica) nos valores de campo onde esta condi¸c˜ao ´e satisfeita. Nesses campos comensur´aveis, os v´ortices podem formar uma rede altamente ordenada onde as intera¸c˜oes v´ortice-v´ortice que reduzem o ancoramento efetivo s˜ao minimizadas. Usando simula¸c˜oes dedinˆamicamolecular,analisamosasconfigura¸c˜oesdosv´orticeseosefeitosdepinning artificialnadinˆamicadev´orticesemumfilmefinosupercondutordotipoII,comumadistribui¸c˜ao peri´odica de centros de pinning. A dinˆamica de v´ortices e suas configura¸c˜oes estruturais, foram simuladas usando o algoritmo de dinˆamica de Langevin. As intera¸c˜oes entre v´ortices foram modeladas dentro da aproxima¸c˜ao de London com condi¸c˜oes de contorno peri´odicas. Na parte inicial do estudo, calculamos as configura¸c˜oes de equil´ıbrio para a rede de v´ortices, encontrando resultados similares aos estudados em trabalhos anteriores. Inclusive, observamos em nossas simula¸c˜oes que o n´umero de satura¸c˜ao dos centros de ancoragem, i.e. o n´umero m´aximo de v´ortices aprisionados por cada centro, ´e fun¸c˜ao do campo externo. de aprisionamento. Esse estudo revela que os tipos de comensurabilidades encontradas nesse problema dinˆamico s˜ao, em geral, diferentes daqueles encontrados no problema est´atico. Portanto, a pr´atica usual na literatura de se inferir sobre as configura¸c˜oes est´aticas dos v´ortices a partir de medidas de magnetorresistˆencia deve ser revista. / Recent progress in manufacturing of nanostructures provides the possibility to produce thin films containing artificial defects as pinning sites with well-defined size, geometry and spatial arrangement. The study of the introduction of a regular arrangement of defects in type II superconducting thinfilmshasbeenactivelydevelopedfromatheoreticalandexperimentalpointofview,ononeside due to the richness of static and dynamic behaviors that it presents and, second, by understanding themechanismstostabilizeandanchorthenetworkofvorticesagainstexternaldrivingforces. One ofthemostremarkablephenomenaofthesesystemsiscalledmatching effectwhichoccurswhenthe number of vortices is a multiple integer of the number of pinning centers, with peaks observed in the cr´ıtical current (static response) or the attenuation of the vortices mobility (dynamic response) values in field where this condition is satisfied. These measurable fields, the vortices can form a highly ordered network where the vortex-vortex interactions that reduce the effective anchoring are minimized. Using molecular dynamics simulations, we analyzed the settings of the vortices and the effects of artificial pinning at the dynamics of vortices in a type II superconducting thin film with a periodic distribution of pinning centers. The dynamics of vortices and their structural configurations were simulated using the Langevin dynamics algorithm. hm. The interactions between vortices were modeled using London’s approach with periodic boundary conditions. In the early part of the study, we calculated the balance settings for the vortex network, finding results similar to those studied in previous works. In fact, we observed in our simulations that the number of saturation of the anchoring centers, i.e. the maximum number of vortices trapped by each center, is a function of the external field. This result had already been predicted in calculations performed within the Ginzburg-Landau formalism. Here, we show that the same effect can be reproduced at the London scheme. In the second part of the study, we analyzed the dynamics when an external force is applied in the longitudinal direction relative to the symmetry of the network of traps. We show that this system displays dynamic commensurability effects when the settings of the vortices coincide with the periodicity of the arrangement, through the magnetoresistance curves that have a number of features in the different fields of matching. Certain field values, it falls in tension are absent due to the particular configuration of vortices and the interaction between interstitial vortices with the vortices occupying the pinning centers. This study shows that the types of measurability found in this dynamic problem are generally different from those found in the static problem. Therefore, the usual practice in the literature to infer the static settings of vortices from magnetoresistance measures should be reviewed.

O processamento em escala laboratorial de soluÃÃes sÃlidas, procedentes dos sistemas Fe2O3/CuO/TiO2 e Fe2O3/Cr2O3, dos seus compÃsitos, e o estudo das propriedades estruturais e de transporte estabelecem o tema principal do trabalho. As granadas ferrimagnÃticas despertam manifesto interesse quanto ao seu emprego em dispositivos aplicÃveis a sistemas de telecomunicaÃÃo operantes nas microondas, sobretudo, em funÃÃo das propriedades dielÃtricas e magnÃticas adequadas. Devido à semelhanÃa estequiomÃtrica, e com a finalidade de se obter materiais com propriedades similares, foram elaborados dois meios magneto-dielÃtricos: (Fe1/4Cu3/8Ti3/8)2O3, um titanato de cobre e ferro, e (Fe5/8Cr3/8)2O3, um Ãxido especÃfico de ferro e cromo. Estas soluÃÃes sÃlidas substitucionais foram sintetizadas por reaÃÃo de estado sÃlido. O processamento avanÃou envolvendo tratamentos mecÃnico e tÃrmico. Foram preparados espÃcimes pulverulentos e com configuraÃÃo definida. A estrutura cristalina dos espÃcimes foi identificada por difraÃÃo de raios-X. Os dados de difraÃÃo de raios-X por policristais foram refinados pelo emprego do mÃtodo de Rietveld. Fez-se uso da espectroscopia MÃssbauer para realizar a sondagem do ferro presente na estrutura cristalina. A morfologia dos espÃcimes, dispostos como peÃas cilÃndricas rÃgidas, foi explorada por Microscopia EletrÃnica de Varredura, assistida por microssonda EDX, para anÃlise quÃmica elementar. Por espectroscopia dielÃtrica foram investigadas as propriedades dielÃtricas permissividade dielÃtrica relativa e fator de perda dielÃtrico e a propriedade de transporte condutividade elÃtrica. As propriedades dielÃtricas e de transporte foram analisadas em funÃÃo da freqÃÃncia, a temperatura ambiente, numa faixa compreendida entre 100 Hz e 40 MHz. Dos dados por difraÃÃo de raios-X, alÃm da identificaÃÃo dos materiais avaliados, foram extraÃdas, apÃs refinamento estrutural, informaÃÃes cristalogrÃficas, no caso das soluÃÃes sÃlidas individuais, e sua quantificaÃÃo, no caso dos compÃsitos por elas constituÃdos. Pela espectroscopia MÃssbauer foram confirmados o estado de oxidaÃÃo do ferro presente nos materiais analisados, a geometria do sÃtio cristalino no qual està presente, a natureza magnÃtica das amostras, e seu provÃvel ordenamento, alÃm da quantificaÃÃo realizada em funÃÃo da quantidade de ferro presente nos compÃsitos. A morfologia dos materiais Ã, em geral, caracterizada pela diversidade de formas e tamanhos dos grÃos, bem como sua disposiÃÃo no artefato explorado. A anÃlise quÃmica elementar forneceu resultados quantitativos acerca dos elementos presentes nos meios investigados. Pela resposta observada na faixa de freqÃÃncia percorrida, ficou evidenciada uma regiÃo de dispersÃo, caracterÃstica do processo de polarizaÃÃo dipolar. Os resultados das propriedades dielÃtricas para as fases sintetizadas mostraram-se parcialmente antagÃnicos: a fase IB100 apresentou a maior permissividade dielÃtrica relativa, porÃm, maior fator de perda dielÃtrica em relaÃÃo à fase IC100, que por sua vez apresentou a menor permissividade dielÃtrica relativa entre todos os materiais investigados. Para os compÃsitos, formados pela mistura aleatÃria de quantidades especÃficas das duas fases sintetizadas, foi evidenciado um comportamento nÃo linear, de forma que estes nÃo representam apenas o reflexo das respostas observadas para as fases individualmente. A fase IB100, em virtude da constante dielÃtrica observada, à o material com maior potencial para aplicaÃÃes em altas freqÃÃncias.

New magnetocaloric Heusler alloys with larger magnetocaloric effects need to function in relatively low applied magnetic fields ≤ 1 T. Therefore, the emphasis of this Ph.D. thesis was to understand how the first order magnetostructural transformation in Mn-rich Ni-based rare-earth free magnetocaloric Heusler alloys works and to use this understanding for the design of new Mn-rich Ni-based rare-earth free magnetocaloric Heusler alloys. In this context, the rare-earth free, non-toxic, and environmentally friendly Heusler series: Ni2−xMn1+xSn, Mn50Ni50−ySny, and Ni-(Co-)Mn-In were systematically studied. In detail, it pointed out that in the Heusler series Ni2−xMn1+xSn, the structure and the disorder character can be predicted by using simple rules. On the other hand, an isoplethal section of the Heusler series Mn50Ni50−ySny was derived, which is very useful for the design of new magnetocaloric materials. In addition to it, in the Heusler alloy Ni49.9Mn34.5In15.6 a large saturated magnetic moment and a reversible magnetocaloric effect at its purely second order magnetic phase transition was present, which is in reasonable agreement with ab initio calculations. Finally, the effect of post-annealing on the Heusler alloy Ni45.2Co5.1Mn36.7In13 revealed that the magnetocaloric effect could be tuned and improved significantly. Consequently, this work shows that the Heusler alloys are promising candidates for magnetocaloric applications.

L'objectif principal de ce travail est le développement d'une équation d’état précise pour la détermination des propriétés thermodynamique de mélange de gaz riche en gaz acides (CO2, H2S) contenant des hydrocarbures et autres gaz (impuretés) comme N2, O2, Ar, etc présente lors du stockage du CO2 (CCS). Après comparaisons avec des données expérimentales, nous avons retenu le modèle SAFT-VR Mie qui prédit de manière satisfaisante les masses volumiques pour les composés purs et les équilibres entre phases. Trois types de propriétés de transport ont également été prédites avec le modèle thermodynamique SAFT-VR Mie associé avec deux autres modèles de prédiction des propriétés de transport (TRAPP et DGT). La prédiction de ces propriétés de transport (viscosité et tension superficielle) repose sur une estimation la plus précise possible des masses volumiques. Pour compléter les banques données expérimentales, les équilibres liquide-vapeur concernant le système binaire H2S-Ar ont été déterminés à l'aide d'un dispositif de mesure dont la méthode technique repose sur la méthode "statique analytique" avec échantillonnage des phases (échantillonneur capillaire ROLI). Déplus, à l'aide d'un densimètre à tube vibrant, les masses volumiques de cinq systèmes binaires (H2S - hydrocarbures (méthane, éthane et propane) ont été mesurées. Les masses volumiques d'un système ternaire (CO2/CH4/H2S) et les masses volumiques et les viscosités d'un mélange multi-constituant riche en CO2 ont aussi été mesurées. Les données sont parfaitement représentées par les modèles développés au cours de cette thèse. / The main aim of this research is to develop a thermodynamic model from an accurate equation of state (EoS) for CO2, hydrocarbons and other gases as N2, O2, Ar, etc. The SAFT-VR Mie EoS was selected to study the phase behaviour and transport properties of mixtures related to carbon capture and storage (CCS). In order to asses this new version of SAFT, several equations of state have been compared (PR, SRK and PC-SAFT). SAFT-VR Mie EoS provides very good density predictions for pure component and binary systems according to the comparative study carried out. Therefore, three transport properties were modelled with SAFT-VR Mie and two models based on density predictions from the EoS. Thus, density, viscosity and interfacial tension (IFT) of CO2-rich systems were calculated by this SAFT-EoS (density), TraPP model (viscosity) and DGT (IFT), in the framework of CCS. Some experimental work was done, in order to extend the available literature data. Isothermal vapor-liquid equilibrium of H2S-Ar binary system was determined at three temperatures from 258 to 288 K. Densities of five binary systems of H2S with methane, ethane and propane were measured continuously at 3 temperatures (253, 273 and 293K) and at pressures up to 30MPa. Following the same technique, the density of the ternary system 42%CO2, 40%CH4 and 18%H2S was measured at pressures ranging from 0.2 to 31.5MPa and at 6 temperatures between 253 and 353K. Densities and viscosities of a multicomponent CO2-rich with 50% of impurities were measured at 5 temperatures between 283 and 423 K and at pressures up to 150 MPa.

This master’s thesis is focused on the subject of graphene modified with atomic hydrogen and its electronic transport properties. Structural and electronic properties of graphene and hydrogenated graphene are compared in the theoretical part of the thesis. The Raman spectroscopy technique is described, including characterization of typical Raman spectra of both unmodified and modified graphene. Samples used during experimental part of the thesis are prepared via laser and electron lithography, and are set to be measured in a vacuum chamber. Subsequently, electronic transport properties are measured before and after hydrogen modification of graphene. Finally, hydrogenated graphene is irradiated using electron beam and changes in its structure are analyzed with Raman spectroscopy techniques.

During neural activity, action potentials travel down axons, generating effective charge current pulses, which are central in neuron-to-neuron communication. Consequently, said current pulses generate associated magnetic fields with amplitudes on the order of picotesla (pT) and femtotesla (fT) and durations of 10’s of ms. Magnetoencephalography (MEG) is a technique used to measure the cortical magnetic fields associated with neural activity. MEG limitations include the inability to detect signals from deeper regions of the brain, the need to house the equipment in special magnetically shielded rooms to cancel out environmental noise, and the use of superconducting magnets, requiring cryogenic temperatures, bringing opportunities for new magnetic sensors to overcome these limitations and to further advance neuroscience. An extraordinary magnetoresistance (EMR) tunable graphene magnetometer could potentially achieve this goal. Its advantages are linear response at room temperature (RT), sensitivity enhancement owing to combination of geometric and Hall effects, microscale size to place the sensor closer to the source or macroscale size for large source area, and noise and sensitivity tailoring. The magnetic sensitivity of EMR sensors is, among others, strongly dependent on the charge mobility of the sensing graphene layer. Mechanisms affecting the carrier mobility in graphene monolayers include interactions between the substrate and graphene, such as electron-phonon scattering, charge impurities, and surface roughness. The present work reviews and proposes a material set for increasing graphene mobility, thus providing a pathway towards pT and fT detection. The successful fabrication of large-size magnetic sensors employing CVD graphene is described, as well as the fabrication of trilayer magnetic sensors employing mechanical exfoliation of h-BN and graphene. The magneto-transport response of CVD graphene Hall bar and EMR magnetic sensors is compared to that obtained in equivalent trilayer devices. The sensor response characteristics are reported, and a determination is provided for key performance parameters such as current and voltage sensitivity and magnetic resolution. These parameters crucially depend on the material's intrinsic properties. The Hall cross magnetic sensor here reported has a magnetic sensitivity of ~ 600 nanotesla (nT). We find that the attained sensitivity of the devices here reported is limited by contaminants on the graphene surface, which negatively impact carrier mobility and carrier density, and by high contact resistance of ~2.7 kΩ µm at the metallic contacts. Reducing the contact resistance to < 150 Ω µm and eliminating surface contamination, as discussed in this work, paves the way towards pT and ultimately fT sensitivity using these novel magnetic sensors. Finite element modeling (FEM) is used to simulate the sensor response, which agrees with experimental data with an error of less than 3%. This enables the prediction and optimization of the magnetic sensor performance as a function of material parameters and fabrication changes. Predictive studies indicate that an EMR magnetic sensor could attain a sensitivity of 1.9 nT/√Hz employing graphene with carrier mobilities of 180,000 cm²/Vs, carrier densities of 1.3×10¹¹ cm^-2 and a device contact resistance of 150 Ω µm. This sensitivity increments to 443 pT/√Hz if the mobility is 245,000 cm²/Vs, carrier density is 1.6×10¹⁰ cm^-2, and a lower contact resistance of 30 Ω µm. Such devices could readily be deployed in wearable devices to detect biomagnetic signals originating from the human heart and skeletal muscles and for developing advanced human-machine interfaces.

Ce travail de thèse porte sur l’élaboration et la caractérisation des propriétés physiques et chimiques d’une nouvelle famille de composés thermoélectriques, et plus particulièrement le composé BiCuSeO. Les composés de cette famille, dite 1111, présentent une structure en couche de type ZrCuSiAs. L’une des particularités de cette structure est la nature distincte des couches qui la composent, la couche Bi2O2 étant décrite comme isolante tandis que la couche Cu2Se2 est appelée couche conductrice. L’étude approfondie du composé BiCuSeO montre qu’en dépit d’un facteur de puissance (S²σ) relativement modéré, ce composé est un matériau thermoélectrique prometteur, notamment à haute température. En effet, BiCuSeO présente une conductivité thermique remarquablement faible, qui permet d’atteindre des facteurs de mérite relativement élevés. De plus, BiCuSeO présente de nombreuses voies d’améliorations possibles. L’une d’elle concerne l’étude d’un dopage aliovalent sur le site du bismuth. L’analyse des résultats a montré que l’insertion d’un élément divalent permet d’optimiser la concentration des porteurs de charges, entrainant ainsi une forte augmentation du facteur de mérite du composé. Une autre voie possible d’exploration est l’étude de l’influence de l’ion chalcogène, au travers notamment de la substitution du sélénium par le tellure, avec l’obtention d’une solution solide complète BiCuSe(1-x)Te(x)O. L’étude des propriétés électriques des composés de cette série a permis de mettre en évidence la présence d’une transition métal – semi-conducteur – métal pour les fractions de tellure inférieures à 0.5. Ainsi, bien que l’influence du tellure sur le facteur de puissance soit relativement limitée en raison de cette anomalie, des résultats intéressants ont été obtenus pour les fractions de tellure élevées. Par ailleurs, des problématiques autour d’une méthode de synthèse alternative du matériau ainsi que sa stabilité sous air sont également abordées dans ce travail. / This thesis addresses the issues of the elaboration and the characterization of the chemical and physical properties of a new family of thermoelectric materials, the oxychalcogenides with the general formula BiCuSeO. This compound, called 1111, cristallises in the ZrCuSiAs structure-type. One feature of this structure lies in the fact that the layers are considered as electronically distinct: the Bi2O2 layers are described as the insulating layers whereas the chalcogenide layers Cu2Se2 are presented as the conductive ones. The study of BiCuSeO exhibits that in spite of a relatively moderate power factor (S²σ), this compound is very promising as possible thermoelectric material, especially at high temperature. Indeed, BiCuSeO shows a remarkably low thermal conductivity, which can achieve relatively high figures of merit. In addition, BiCuSeO offers many ways for improvement. One of them concerns the study of aliovalent doping on the bismuth site. The results showed that the insertion of a divalent element optimizes the charge carriers concentration, leading to a sharp increase in the figure of merit of the compound. Another possible way of exploration lies the study of the influence of the chalcogen ion, notably through the substitution of selenium and tellurium, with a complete solid-solution BiCuSe(1-x)Te(x)O. The study of the electrical properties of this solid solution has highlighted the presence of a metal - semiconductor - metal transition for tellurium fractions below 0.5. Thus, although the influence of tellurium on the power factor is relatively limited due to this anomaly, interesting results were obtained for the high tellurium fractions. In addition, issues around an alternative method of synthesis of the material and its stability in air are also discussed in this work.

No description available.