We have grown Ga1-xMnxN films on c-sapphire substrate by plasma-assisted MBE with different Mn fluxes. The films are characterized by scanning electron microscopy (SEM), energy dispersive spectrometer (EDS), electron backscatter diffraction (EBSD), high¡Vresolution X-ray diffraction (HR-XRD), Raman scattering, photoluminescence (PL), cathodoluminescence (CL), transmission spectra, reflection spectra and X-ray photoelectron spectroscopy (XPS). The SEM images show films thickness between 550 to 850 nm and EBSD indicates samples normal direction is c-axis. EDS spectra show the Mn is present in GaMnN samples. According to XRD and Raman scattering, Mn element occupying Ga site on GaN and Mn-N clusters phase coexist on films. From transmission and reflection spectra, stronger absorption at about 1.5 eV and 1.8 eV to 3.4 eV absorption band are found. The PL and CL show GaN band gap at 3.4 eV and blue band from 2.4 eV to 3.3 eV maybe due to defect level. Finally, the XPS spectra indicate Mn acceptor level is contributed to Mn+2 or Mn+3 states.

Made available in DSpace on 2014-06-11T19:31:04Z (GMT). No. of bitstreams: 0 Previous issue date: 2011-02-17Bitstream added on 2014-06-13T20:21:45Z : No. of bitstreams: 1 leite_dmg_dr_bauru.pdf: 3640633 bytes, checksum: adf6650360687a658c11b1cc1b69b693 (MD5) / Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP) / A recente busca por semicondutores magnéticos diluídos com propriedades magnéticas de interesse motivou este trabalho de crescimento de filmes de Ga1-xMnxN pelas técnicas de sputtering e epitaxia da fase de vapor de organometálicos (MOVPE). Os filmes são caracterizados estruturalmente por medidas de difração de raio X e microscopia eletrônica de transmissão, opticamente por transmitância óptica e espalhaçamento Raman, e magneticamente por medidas magnetização versus campo aplicado e versus temperatura. As principais diferenças entre os filmes de GaMnN preparados por sputerring e MOVPE referem-se à microestrutura e ao conteúdo de Mn: os primeiros são policristalinos e apresentam conteúdo de Mn até 9%, enquanto os últimos são monocristalinos com concentração de Mn até 1%. A alta concentraçao de Mn nos filmes crescidos por sputtering é possivelmente responsável pelo surgimento coletivo destes íons de Mn nas medidas magnéticas. Esse comportamento coletivo se identifica a partir de contribuição paramagnética de domínios isolados com alto vapor de momento magnético, o que se mostra consistente com a microestrutura apresentada por estes filmes. A alta concentração de Mn nos filmes preparados por sputtering também se mostra responsável por intensa absorção óptica abaixo da energia do gap, sendo esta relacionada a transições eletrônicas entre os estados localizados do Mn e as bandas de valência e condução do GaN. O contraste entre as propriedades dos filmes de GaMnN produzidos por sputtering e por MOVPE possibilita então um entendimento mais abrangente dos aspectos da incorporação de Mn no GaN e suas respectivas características estruturais, ópticas e magnéticas. Esse entendimento é importante para delinear a otimização deste material visando propriedades magnéticas de interesse / The current search for dilluted magnetic semiconductors with interesting magnetic properties has motivated the present work on growing GaMnN films by sputerring and metalorganic vapor phase epitaxy (MOVPE) techniques. The films are characterized by X-ray diffraction, transmission electron microscopy, optical transmission, Raman scattering, and by magnetization measurements. The main differece between the GaMnN grown by sputtering and those grown by MOVPE relates to their microstructure (polycrystalline/monocrystalline) and Mn content (up to 9%/1% respectively). The high Mn content in GaMnN samples grown by sputtering is probably responsible for a collective response on the magnetic measurements. This collective Mn response is identified as a high magnetic moment contribution which is consistent with sample microstructure. In the sputtered samples, the high Mn content is also responsible for strong subbandgap optical absorption related to eletronic transitions involving Mn states and the valence and conduction bands of GaN. The comparison between the properties of GaMnN films grown by different techniques is important in order to get a better understanding about the Mn incorporation in GaN. This understanding been important to define the next steps regarding the optimization of this material

Orientador: José Humberto Dias da Silva / Banca: Carlos Frederico de Oliveira Graeff / Banca: Antonio Ricardo Zanatta / O Programa de Pós-Graduação em Ciência e Tecnologia de Materiais, PosMat, tem caráter institucional e integra as atividades de pesquisa em materiais de diversos campi da Unesp / Resumo: A recente descoberta de propriedades ferromagnéticas em alguns semicondutores magnéticos diluídos (DMS) trouxe a esta classe de materiais um grande potencial para aplicações em dispositivos de controle de spin. Um DMS é basicamente formado por um semicondutor dopado por íons magnéticos, os quais têm o papel de criar um momento magnético local e também, em algumas situações, de introduzir portadores livres no material. Entre os DMSs conhecidos, o 'GA IND.1-x'MN IND.XN' surge como o mais forte candidato a aplicações práticas por apresentar até o momento a mais alta temperatura de transição ferromagnética ('T IND.C' 'DA ORDEM DE' 400 k). Até o presente, os filmes de 'GA IND.1-x'MN IND.XN' com propriedades ferromagnéticas relatados na literatura foram preparados por epitaxia por feixe molecular (MBE). Neste trabalho, descrevemos a preparação de filmes nanocristalinos de 'GA IND.1-x'MN IND.XN' com diferentes conteúdos de Mn (0,00 'MENOR' x 'MENOR' 0,18) pela técnica de RF-magnetron sputtering reativo. Analisamos os efeitos da incorporação de Mn na estrutura e nas propriedades ópticas destes filmes através de medidas de difração de raios-X e de absorção óptica entre o ultravioleta (6,5 eV) e infravermelho próximo (1,4 eV). Os resultados apontam um aumento do parâmetro de rede e do índice de refração, uma diminuição do gap ótico e um aumento da densidade de estados de defeitos no interior do gap conforme se aumenta o conteúdo de Mn nos filmes de 'GA IND.1-x'MN IND.XN' preparados por sputtering. Estes resultados são semelhantes aos reportados para a incorporação de Mn em filmes monocristalinos de 'GA IND.1-x'MN IND.XN' com propriedades ferromagnéticas preparados por MBE. / Abstract: The recent discoveries related to the ferromagnetic properties in some diluted magnetic semiconductors (DMS) have attracted considerable attention on this class of material due to their potential application on spin control devices. A DMS is basically formed by a semiconductor doped with magnetic ions with the purpose of creating local magnetic moments and, in some situations, to introduce free carriers in the material. Among the known DMSs, 'GA IND.1-x'MN IND.XN' is the one with the highest ferromagnetic transition temperature ('T IND.C' 'DA ORDEM DE' 400 k), and it is consequently on of the stronger candidates for practical applications. Until now, the 'GA IND.1-x'MN IND.XN' films with ferromagnetic properties described in the literature were prepared by molecular beam epitaxy (MBE). In this work, we report the preparation of nanocrystalline 'GA IND.1-x'MN IND.XN' films (0,00 'MENOR' x 'MENOR' 0,18) by reactive RF-magnetron sputtering technique. We analyzed the Mn incorporation effects on structure and optical properties of the films by X-ray diffraction measurements and optical absorption between UV (6,5 eV) and near infrared (1,4 eV). The results show the increase of the lattice parameters and of the refractive index, a decrease of the optical gap and a increase of defect states in the gap when Mn concentration is increased. These results are similar to those reported for Mn incorporation in monocrystalline 'GA IND.1-x'MN IND.XN' films prepared by MBE with ferromagnetic properties. / Mestre

Ce manuscrit présente une étude sur les ondes de spin de vecteur d'onde nul par le moyen de la rotation Kerr résolue en temps. Les ondes de spin sont générées dans un puits quantique CdMnTe dopé n, ce qui introduit de la complexité dans le système. Le résultat principal de cette étude est l'apparition d'un anticroisement de mode d'excitation du gaz d'électron appelé onde de spin et du mode d'excitation des spins localisés sur les sites des ions magnétiques. Cet effet est provoqué par le couplage des deux systèmes de spin par l'interaction d'échange. On accède alors à la mesure de la polarisation du gaz bidimensionnel d'électrons qui ce compare très bien à la théorie tenant compte de l'augmentation de la polarisation par les effets à N-corps. Une partie de ce manuscrit est consacré à la mise en place expérimentale de la rotation Kerr résolue en temps. On étudie ensuite l'onde de spin pour les champs magnétiques hors résonance. On montre que le temps de relaxation de l'onde n'est pas encore complètement compris, même si nous décrivons un modèle de relaxation inhomogène. Puis nous étudions finalement la résonance où nous montrons que la description habituelle en champs moyen ne convient pas, et nous proposons un modèle au delà de cette approximation qui permet une mesure de la polarisation du gaz bidimensionnel d'électrons en accord avec la théorie. / This manuscript present a study of nul wave vector spin flip waves by time resolved Kerr rotation. Spin flip waves are generated in a n doped CdMnTe quantum well, increasing the complexity of the system. The main result of this study is the apparition of an anticrossing between the excitation mode of the electron gaz called spin flip wave and the excitation mode of localized spin on magnetic ions. This effect is caused by the coupling of the two spin sytem by the exchange interaction. We acces then to the gaz spin polarization which is compared to theorie explaining the enhancement of the polarization by many-body effects. A part of this manuscript is dedicated to the experimental set-up of the time resolved Kerr rotation. Next, we study the spin flip wave for magnetic field below the resonance. We show that the relaxation time of the spin wave is not well understand even if we describe a model of inhomogeneous relaxation. Finally we study the resonance and we show that the mean field description don't work and we propose a model beyond the mean field which allow a measurement of the spin polarization of electron gas in agreement with the theorie.

The roles of hydrogen induced defects in pure ZnO has been studied extensively. However, in a transition metal, such as Co, doped ZnO thin films the effect of hydrogen in electric conduction and magnetic coupling is still unclear and needs further study. Recently model predicts that hydrogen can be a shallow donor as well as an agent to induce ferromagnetism coupling between two adjacent Co ions which substitute the Zn sites at room temperature in a ZnO sample with a high Co doping ratio. However, the experimental supports is rare. In this study, Co-doped(5%) ZnO films are grown by a RF-magnetron sputtering system on glass substrate at room temperature. The growth condition is fixed for RF power in 200W, working press of 70 mtorr and various mixing ratio of H2/Ar+H2 gas. The crystal structure, electric and optical properties and the influence of vacuum annealing on the samples are studied. In this research, we found that the doping of hydrogen in Co-doped ZnO thin films truly increases the electric conductivity which is proportional to the H2/(Ar+H2) ratio. When the ratio of hydrogen is low, the (002) peak taken by a Glazing Angle X-ray Diffractometer dominates, while increasing hydrogen ratio other diffraction peaks appear, indicating an enhancement of crystal structure in all directions, and grain sizes and unit cell volume decrease. From the optical transmittance measurement, it is found that the color of films turned into metallic like and the optical band gap increases linearly with H2 ratio which can be attributed to the Burstein-Moss effect that corresponds to the increasing of carriers in the conduction band by doping of H2. The transmittance data provides the information of the ratio of crystalline and amorphous, which can also be correlated to the AFM results. When the H2 ratio is higher than 30%, more crystals and larger sizes of grains were formed in the films, such that carriers did not need to pass grain boundaries so frequently and experienced less scattering that was actually improve the electric conductivity. The electric conductivity can be even improved by post annealing in H2 environment. Moreover, the Magnetic circular dichroism (MCD) measurement shows that the Co2+ ions does truly substitute on Zn sited in Td symmetry during thin film deposition. The resistance measurement as a function of temperature found the hydrogenated Co-doped thin films are semiconductor conductive. More works are needed to determine the magnetization, identify second phases and Vo by SQUID and X-ray photoelectron spectroscopy.

Made available in DSpace on 2014-06-11T19:23:29Z (GMT). No. of bitstreams: 0 Previous issue date: 2007-02-02Bitstream added on 2014-06-13T18:50:38Z : No. of bitstreams: 1 leite_dmg_me_bauru.pdf: 1278982 bytes, checksum: f2b696ae90b2738246ee3c7750b37751 (MD5) / A recente descoberta de propriedades ferromagnéticas em alguns semicondutores magnéticos diluídos (DMS) trouxe a esta classe de materiais um grande potencial para aplicações em dispositivos de controle de spin. Um DMS é basicamente formado por um semicondutor dopado por íons magnéticos, os quais têm o papel de criar um momento magnético local e também, em algumas situações, de introduzir portadores livres no material. Entre os DMSs conhecidos, o 'GA IND.1-x'MN IND.XN' surge como o mais forte candidato a aplicações práticas por apresentar até o momento a mais alta temperatura de transição ferromagnética ('T IND.C' 'DA ORDEM DE' 400 k). Até o presente, os filmes de 'GA IND.1-x'MN IND.XN' com propriedades ferromagnéticas relatados na literatura foram preparados por epitaxia por feixe molecular (MBE). Neste trabalho, descrevemos a preparação de filmes nanocristalinos de 'GA IND.1-x'MN IND.XN' com diferentes conteúdos de Mn (0,00 'MENOR' x 'MENOR' 0,18) pela técnica de RF-magnetron sputtering reativo. Analisamos os efeitos da incorporação de Mn na estrutura e nas propriedades ópticas destes filmes através de medidas de difração de raios-X e de absorção óptica entre o ultravioleta (6,5 eV) e infravermelho próximo (1,4 eV). Os resultados apontam um aumento do parâmetro de rede e do índice de refração, uma diminuição do gap ótico e um aumento da densidade de estados de defeitos no interior do gap conforme se aumenta o conteúdo de Mn nos filmes de 'GA IND.1-x'MN IND.XN' preparados por sputtering. Estes resultados são semelhantes aos reportados para a incorporação de Mn em filmes monocristalinos de 'GA IND.1-x'MN IND.XN' com propriedades ferromagnéticas preparados por MBE. / The recent discoveries related to the ferromagnetic properties in some diluted magnetic semiconductors (DMS) have attracted considerable attention on this class of material due to their potential application on spin control devices. A DMS is basically formed by a semiconductor doped with magnetic ions with the purpose of creating local magnetic moments and, in some situations, to introduce free carriers in the material. Among the known DMSs, 'GA IND.1-x'MN IND.XN' is the one with the highest ferromagnetic transition temperature ('T IND.C' 'DA ORDEM DE' 400 k), and it is consequently on of the stronger candidates for practical applications. Until now, the 'GA IND.1-x'MN IND.XN' films with ferromagnetic properties described in the literature were prepared by molecular beam epitaxy (MBE). In this work, we report the preparation of nanocrystalline 'GA IND.1-x'MN IND.XN' films (0,00 'MENOR' x 'MENOR' 0,18) by reactive RF-magnetron sputtering technique. We analyzed the Mn incorporation effects on structure and optical properties of the films by X-ray diffraction measurements and optical absorption between UV (6,5 eV) and near infrared (1,4 eV). The results show the increase of the lattice parameters and of the refractive index, a decrease of the optical gap and a increase of defect states in the gap when Mn concentration is increased. These results are similar to those reported for Mn incorporation in monocrystalline 'GA IND.1-x'MN IND.XN' films prepared by MBE with ferromagnetic properties.

Orientador: José Humberto Dias da Silva / Banca: Jair Scarminio / Banca: Alexys Bruno Alfonso / Banca: Pascoal José Giglio Pagliuso / Banca: Luis Vicente de Andrade Scalvi / O Programa de Pós-Graduação em Ciência e Tecnologia de Materiais, PosMat, tem caráter institucional e integra as atividades de pesquisa em materiais de diversos campi da Unesp / Resumo: A recente busca por semicondutores magnéticos diluídos com propriedades magnéticas de interesse motivou este trabalho de crescimento de filmes de Ga1-xMnxN pelas técnicas de sputtering e epitaxia da fase de vapor de organometálicos (MOVPE). Os filmes são caracterizados estruturalmente por medidas de difração de raio X e microscopia eletrônica de transmissão, opticamente por transmitância óptica e espalhaçamento Raman, e magneticamente por medidas magnetização versus campo aplicado e versus temperatura. As principais diferenças entre os filmes de GaMnN preparados por sputerring e MOVPE referem-se à microestrutura e ao conteúdo de Mn: os primeiros são policristalinos e apresentam conteúdo de Mn até 9%, enquanto os últimos são monocristalinos com concentração de Mn até 1%. A alta concentraçao de Mn nos filmes crescidos por sputtering é possivelmente responsável pelo surgimento coletivo destes íons de Mn nas medidas magnéticas. Esse comportamento coletivo se identifica a partir de contribuição paramagnética de domínios isolados com alto vapor de momento magnético, o que se mostra consistente com a microestrutura apresentada por estes filmes. A alta concentração de Mn nos filmes preparados por sputtering também se mostra responsável por intensa absorção óptica abaixo da energia do gap, sendo esta relacionada a transições eletrônicas entre os estados localizados do Mn e as bandas de valência e condução do GaN. O contraste entre as propriedades dos filmes de GaMnN produzidos por sputtering e por MOVPE possibilita então um entendimento mais abrangente dos aspectos da incorporação de Mn no GaN e suas respectivas características estruturais, ópticas e magnéticas. Esse entendimento é importante para delinear a otimização deste material visando propriedades magnéticas de interesse / Abstract: The current search for dilluted magnetic semiconductors with interesting magnetic properties has motivated the present work on growing GaMnN films by sputerring and metalorganic vapor phase epitaxy (MOVPE) techniques. The films are characterized by X-ray diffraction, transmission electron microscopy, optical transmission, Raman scattering, and by magnetization measurements. The main differece between the GaMnN grown by sputtering and those grown by MOVPE relates to their microstructure (polycrystalline/monocrystalline) and Mn content (up to 9%/1% respectively). The high Mn content in GaMnN samples grown by sputtering is probably responsible for a collective response on the magnetic measurements. This collective Mn response is identified as a high magnetic moment contribution which is consistent with sample microstructure. In the sputtered samples, the high Mn content is also responsible for strong subbandgap optical absorption related to eletronic transitions involving Mn states and the valence and conduction bands of GaN. The comparison between the properties of GaMnN films grown by different techniques is important in order to get a better understanding about the Mn incorporation in GaN. This understanding been important to define the next steps regarding the optimization of this material / Doutor

Nous avons étudié la dynamique de spin d'un atome de Mn inséré dans une boite quantique CdTe. Nos résultats montrent que la relaxation de spin du Mn est plus rapide lorsque la boite quantique contient un exciton. Ceci peut permettre une orientation optique du spin du Mn. Le mélange de bande de valence est le paramètre essentiel permettant la relaxation rapide du spin du Mn dans le champ d'échange de l'exciton. Ce mélange de bande de valence est controlé par la forme et les contraintes dans la boite quantique. L'influence de ces paramètres sur la dynamique du pompage optique a été analysée en détail. Nos simulations du pompage optique sont en bon accord avec les expériences. La dynamique cohérente d'un Mn individuel a aussi été étudiée. L'influence sur le pompage optique de la dynamique cohérente du spin électronique et nucléaire est discutée. Nous avons montré que le couplage entre spin électronique et nucléaire peut être contrôlé optiquement permettant une manipulation du spin du Mn. Nous avons finalement montré que la combinaison d'une excitation résonante optique et micro-onde peut être utilisée pour détecter optiquement la résonance magnétique d'un Mn dans une boite quantique CdTe. / We have studied the spin dynamics of an individual Mn atom embedded a CdTe quantum dot. Our results show that the Mn spin relaxation is faster when the quantum dot contains an exciton. This can result in an optical orientation of the Mn spin. The valence band mixing is the critical parameter for the fast relaxation rates of the Mn spin in the exchange field of the exciton. This valence band mixing is controlled by the shape and strain of the quantum dot. The influence of these parameters on the optical pumping dynamics were analyzed in detail. Our simulation of optical pumping are in good agreement with experiments. The coherent dynamics of an individual Mn spin was also investigated. We discussed the influence of the coherent dynamics of the coupled electronic and nuclear spins on the optical pumping. We have shown that optically controlled coupling between electronic and nuclear spins could be used for Mn spin switching. We finally demonstrated that the combination of resonant laser and microwave fields can be used to optically detect the magnetic resonance of a Mn spin in a CdTe quantum dot.

Nous avons étudié la dynamique de spin d'un atome de Mn inséré dans une boite quantique CdTe. Nos résultats montrent que la relaxation de spin du Mn est plus rapide lorsque la boite quantique contient un exciton. Ceci peut permettre une orientation optique du spin du Mn. Le mélange de bande de valence est le paramètre essentiel permettant la relaxation rapide du spin du Mn dans le champ d'échange de l'exciton. Ce mélange de bande de valence est controlé par la forme et les contraintes dans la boite quantique. L'influence de ces paramètres sur la dynamique du pompage optique a été analysée en détail. Nos simulations du pompage optique sont en bon accord avec les expériences. La dynamique cohérente d'un Mn individuel a aussi été étudiée. L'influence sur le pompage optique de la dynamique cohérente du spin électronique et nucléaire est discutée. Nous avons montré que le couplage entre spin électronique et nucléaire peut être contrôlé optiquement permettant une manipulation du spin du Mn. Nous avons finalement montré que la combinaison d'une excitation résonante optique et micro-onde peut être utilisée pour détecter optiquement la résonance magnétique d'un Mn dans une boite quantique CdTe. / We have studied the spin dynamics of an individual Mn atom embedded a CdTe quantum dot. Our results show that the Mn spin relaxation is faster when the quantum dot contains an exciton. This can result in an optical orientation of the Mn spin. The valence band mixing is the critical parameter for the fast relaxation rates of the Mn spin in the exchange field of the exciton. This valence band mixing is controlled by the shape and strain of the quantum dot. The influence of these parameters on the optical pumping dynamics were analyzed in detail. Our simulation of optical pumping are in good agreement with experiments. The coherent dynamics of an individual Mn spin was also investigated. We discussed the influence of the coherent dynamics of the coupled electronic and nuclear spins on the optical pumping. We have shown that optically controlled coupling between electronic and nuclear spins could be used for Mn spin switching. We finally demonstrated that the combination of resonant laser and microwave fields can be used to optically detect the magnetic resonance of a Mn spin in a CdTe quantum dot.

No description available.