Conselho Nacional de Desenvolvimento Científico e Tecnológico / Hybrid nanostructures which integrate two or more technologically interesting physical properties are fundamental for developing new generations of electronic devices. Exhibiting at least two coupled ferroic orders, multiferroics are an outstanding class of multifunctional materials. Compounds which present coupling between ferromagnetism and ferroelectricity are specially interesting. Although natural multiferroics are rarely found, the possibility of obtaining strain-mediated magnetoelectric coupling in composite structures, by integrating magnetostrictive and piezoelectric layers, paves the way to control electric properties by applying magnetic field or to the electric control of magnetism. Nevertheless, most scientific efforts have been on monophasic compounds or bulk composites. Considering the incorporation of magnetoelectric nanostructures in devices, expanding the scope of the magnetoelectric effect and targetting it to different kinds of applications is needed. Besides new characterization techniques, seeking new alternative materials to the lead-based piezoelectrics or oxide-based magnetostrictives is necessary. Recently, a few works using semiconductors such as ZnO and AlN, or amorphous magnetic alloys such as those based on Co, Fe and Ni, have been reported. In spite of not presenting remarkable piezoelectric and magnetostrictive effects, the features of such materials are promising for high frequency applications, for instance. Considering these issues, four independent surveys are presented. Firstly, the origin of the coupling, latest advances and current scenario of the field are reviewed. Then magnetostriction measurements in thin films are addressed by employing a direct technique based on the cantilever-capacitance method. The goals are to study magnetoelastic properties of some materials whose magnetostriction are not found very often in literature, and to check the reliability of this technique for investigating thin films. In this sense, measurements of some amorphous magnetic alloys mainly based on Co, Fe and Ni are performed. Most samples presents larger magnetoelastic response for magnetic field applied along the magnetization easy axis, as opposed to the theoretically expected. Two investigations on aluminum nitride thin films are reported. Firstly, the growth of AlN films onto several different substrates and buffer layers is studied. Films grown onto glass and polyimide show excellent structural properties for eletromechanical systems and flexible electronics applications. Samples with low residual stress on silicon substrates, suitable for incorporating in existing technologies, are obtained. Secondly, bilayers composed by AlN and ferromagnetic films are investigated. In addition to the structural and morphological properties of the AlN films which are checked, the magnetic characterization of the structures also contributes to design multilayers for exploring the magnetoelectric effect. Finally, problems involving electric fields in scanning probe microscopies are adressed. Surface images of AlN piezoelectric films are systematically acquired. Among other major observations, the possibility of getting reliable piezoresponse images of strongly polarized areas as well as of visualizing ferroelastic domains, is demonstrated. Furthermore, a new microscopy for investigating a sample s ferro and piezoelectric properties is proposed, exploring the direct piezoelectric effect. By utilizing acoustic excitation and electrical detection, the potency of this technique is illustrated with measurements on quartz and AlN surfaces. / Nanoestruturas híbridas, integrando duas ou mais propriedades físicas de grande interesse tecnológico, são fundamentais para o desenvolvimento de novas gerações de dispositivos eletrônicos. Uma classe interessante de materiais multifuncionais são os multiferróicos, que exibem pelo menos duas ordens ferróicas acopladas. Dentre eles, os que apresentam acoplamento entre ferromagnetismo e ferroeletricidade despertam interesse especial. Apesar de serem raros de ocorrer naturalmente, a possibilidade de gerar efeito magnetoelétrico em estruturas compósitas, intermediado pela deformação elástica entre camadas magnetostrictivas e piezoelétricas, abre caminho para que seja possível controlar propriedades elétricas aplicando-se campo magnético, ou propriedades magnéticas aplicando-se campo elétrico. Todavia, a maior parte das pesquisas atuais ainda envolve compostos monofásicos ou compósitos em forma massiva. Tendo em vista a incorporação de nanoestruturas magnetoelétricas em dispositivos, é fundamental ampliar a abrangência do efeito magnetoelétrico e direcioná-lo para diferentes tipos de aplicações. Para isto, além de novas técnicas de caracterização, é necessário buscar-se materiais alternativos aos tradicionais piezoelétricos baseados em chumbo e magnetostrictivos baseados em óxidos. Recentemente tem-se encontrado trabalhos pontuais onde são utilizados piezoelétricos semicondutores como ZnO e AlN, e ligas magnéticas amorfas como as baseadas em Co, Fe e Ni. Mesmo sem apresentar efeitos piezoelétrico e magnetostrictivo com magnitudes notáveis, as características destes materiais são promissoras para aplicações envolvendo altas frequências, por exemplo. Neste necessário, são apresentados quatro estudos independentes entre si. Primeiramente, é realizada uma revisão sobre a origem do acoplamento, os últimos avanços e o panorama atual das pesquisas na área. Em seguida, através de uma técnica direta baseada no método do cantiléver-capacitância, aborda-se o problema das medidas de magnetostricção em amostras na forma de filmes finos. Os objetivos são estudar as propriedades magnetoelásticas em alguns materiais que não são frequentemente abordados pela literatura, e avaliar a potencialidade da técnica para a análise de filmes finos. Para isto, são realizadas medidas principalmente em ligas ferromagnéticas amorfas baseadas em Co, Fe e Ni. Para a maioria das amostras analisadas, a resposta magnetoelástica é maior quando o campo magnético é aplicado na direção do eixo de fácil magnetização, de forma contrária à esperada teoricamente. São apresentadas duas investigações envolvendo filmes finos de nitreto de alumínio. Primeiro é estudado o crescimento de filmes de AlN sobre vários substratos e camadas semente. Filmes crescidos sobre vidro e poliimida apresentam excelentes propriedades estruturais para aplicações em sistemas eletromecânicos e eletrônica flexível. Amostras obtidas com baixos valores de tensão residual, sobre substratos de silício, são interessantes para incorporação em tecnologias existentes. Segundo, são investigadas bicamadas de AlN com filmes ferromagnéticos. Além das propriedades estruturais e morfológicas dos filmes de AlN, a análise das características magnéticas das estruturas contribui para o design de multicamadas que exploram o efeito magnetoelétrico. Finalmente, são abordados problemas em medidas de microscopias de varredura por sonda envolvendo campos elétricos. Imagens da superfície de filmes piezoelétricos de AlN foram coletadas sistematicamente. Entre outras observações importantes, demonstra-se que é possível adquirir imagens confiáveis de piezo-resposta em regiões fortemente polarizadas, e visualizar a formação de domínios ferroelásticos. Também é proposta uma nova técnica de microscopia, para investigar as propriedades ferro e piezoelétricas de uma amostra, explorando o efeito piezoelétrico direto. Utilizando excitação acústica e detecção elétrica, o potencial da nova técnica é demonstrado com imagens de superfícies cristalinas de quartzo e AlN.

Magnetostrictive materials belong to an important class of smart magnetic materials which have potential applications as ultrasonic transducers, sensors, actuators, delay lines, energy harvesting devices etc. Although, magnetostrictive property is exhibited by almost all ferro and ferrimagnetic materials, the R-Fe type (R represents rare earth elements) intermetallic compounds display maximum promise owing to the large magnetostriction exhibited by them at ambient temperature. Among the several R-Fe type compounds, Tb-Fe and Sm-Fe alloys are found to exhibit maximum room temperature positive and negative magnetostriction respectively. Recently, Fe-Ga based alloys have gained significant interest as newly emerging magnetostrictive material due to a good combination of magnetic and mechanical properties. These magnetostrictive materials in thin film form are of interests for several researchers both from fundamental and applied perspectives. Currently, many researchers are exploring the possibility of using magnetostrictive thin films in micro- and nano-electromechanical systems (MEMS and NEMS). Three material systems viz. Fe-Ga, Tb-Fe and Sm-Fe in thin film form have been chosen for our investigations. DC magnetron sputtering and e-beam evaporation techniques were used for deposition of these thin films on Si (100) substrates. Several aspects such as evolution of microstructure, film surface morphology, structure and change in film composition with different processing conditions were investigated in detail, as the existing literature could not provide a clear insight. Further, detailed magnetic characterizations of these films were carried out and established a process-structure-property correlation. The thesis is divided into seven chapters. The first chapter presents a brief introduction of magnetostrictive phenomena and the physics behind its origin. A brief history of evolution of magnetostrictive materials with superior properties is also brought out. Introduction to the material systems considered for the present study has also been presented. Discussions on various aspects like crystal structures, magnetic properties, and phase diagrams of these material systems are also included in this chapter. Magnetostriction in thin films and its importance in current technological applications are discussed in short. Further, a summary of existing literature on thin films of these materials has been narrated to highlight the perspective of the work done in subsequent chapters. In addition to this, a clear picture of the grey area for further investigations has been provided. Formulation of detailed scope of work for this study is also provided in this chapter. Details of different experimental techniques used in this study for deposition and characterization of these films are given in chapter 2. In the third chapter of the thesis a detailed study on the structural, microstructural and magnetic properties of Fe-Ga films deposited using dc magnetron sputtering technique are presented. The effect of sputtering parameters such as (i) Ar pressure, (ii) sputtering power, (iii) substrate temperature and (iv) deposition time/film thickness on the magnetic properties of the films are discussed in detail. All the films are found to be polycrystalline in nature with A2 type structure as evidenced from grazing incidence X-ray diffraction (GIXRD) and transmission electron microscope (TEM) studies. Surface morphology of the films are found to be affected with processing conditions considerably. Thermomagnetic behaviour of the films studied using a Superconducting Quantum Interference Device (SQUID) magnetometer under zero field cooled (ZFC) and field cooled (FC) conditions are also presented. The sputtering parameters are also found to influence the magnetic properties of the films through modifications in microstructure, surface morphology and film compositions. Irrespective of the sputtering parameters, room temperature (RT) deposited Fe-Ga films are found to exhibit large magnetic coercively and large saturation magnetic field as compared to the bulk alloy of similar compositions which are not desirable for micromagnetic device applications. A significant improvement in the magnetic properties of the films was obtained in the films deposited at higher substrate temperatures and is correlated with modifications in grain size and film surface roughness. These films are also found to exhibit better magnetostriction than the RT deposited films. Further, the magnetic properties of Fe-Ga films as a function of film thickness in the range 2 – 480 nm are also presented. The nature of variation of coercively with film thickness was correlated with grain size effect and explained successfully with the help of random anisotropy model. In the fourth chapter, studies on the microstructural and magnetic properties of Tb-Fe films were presented. It was reported earlier that TbxFe100-x films exhibit in-plane magnetic anisotropy for the films with x > 42 at.% of Tb and out-of-plane anisotropy for the composition 28 < x < 42. Presence of these anisotropies is technologically important for different applications. We have studied the magnetic properties of Tb-Fe films in these two composition range. TbxFe100-x films with 54  x  59 were prepared using dc magnetron sputtering technique under varying Ar pressure and sputtering power and the details about microstructural and magnetic properties are presented in this chapter. All the films are found to be amorphous in nature. While the composition of the film is found to remain constant with sputtering power, the Fe concentration in the film is found to be depleted with increase in Ar pressure. Magnetic properties are found to change from superparamagnetic to ferromagnetic behaviour with increase in sputtering power. Curie temperature of the films are found to be low (below RT) and is explained based on sperimagnetic ordering of magnetic sub-lattices. The perpendicular magnetic anisotropy (PMA) or out-of-plane anisotropy behaviour of Tb-Fe films were not studied in detail as a function of film thickness. We have successfully prepared TbxFe100-x films with 29  x  40 using e-beam evaporation technique using alloy target composition of TbFe in order to study the PMA behaviour as a function of film thickness. The thickness of the films was varied from 50 to 800 nm. All the films are found to be amorphous and columnar growth structure with fine channels of voids are observed from the TEM studies. Detailed magnetization and thermomagnetic measurements were carried out using SQUID magnetometer at different temperatures. The out-of-plane magnetic coercivity of the films was found to increase with film thickness and then decreases with further increase in thickness. Maximum coercivity of ~ 20 kOe has been obtained for the 400 nm thick film. Magnetic domain patterns were studied using magnetic force microscopy (MFM) technique and the observed magnetic properties are correlated with domain pattern and microstructures. Although there are several reports on device applications of Sm-Fe thin films which exhibit negative magnetostriction, a comprehensive study on the effect of different process parameters on the magnetic properties and its correlation with structure and microstructure is still elusive. Hence, Sm-Fe films were deposited on Si (100) substrate using dc magnetron sputtering technique under varying Ar pressure and sputtering power. Effect of these parameters on the microstructural and magnetic properties of the films was studied in detail and is presented in chapter 5. The curie temperature of the films was found to increase with increase in sputtering power and Ar pressure. This was attributed to increase in film thickness and size of islands (atomic clusters). Coercivity as low as 30 Oe has been achieved in the film deposited at 15 mTorr Ar pressure. The Curie temperature for the films deposited at higher Ar pressure (10 and 15 mTorr) are found to be above RT. Maximum saturation magnetostriction of ~ - 390 -strains has been achieved in the film deposited at 15 mTorr Ar pressure. Rapid thermal processing (RTP) experiments were also carried out to increase the magnetic ordering in the films deposited at low Ar pressure (5 mTorr) by imparting structural ordering. Large improvement in magnetization and Curie temperature of the film was observed after RTA. However, this could be attributed to the formation of nano-crystalline Fe phase as evidenced from the TEM studies and thermomagnetic measurements. An overall summary of the experimental results has been presented in chapter 6. The scope of work for further study in future has also been highlighted in chapter 7.

Dehnungssensoren werden zur Überwachung von sicherheitsrelevanten Bauteilen, besonders in Bauteilen aus faserverstärkten Polymermatrixverbundwerkstoffen eingesetzt. Durch deren Integration in das Bauteilinnere werden sie vor schädigenden mechanischen sowie korrosiven Einwirkungen geschützt. Dies gewährleistet eine zuverlässige sowie dauerhafte Funktion. Verschiedene Ansätze zur Weiterentwicklung integrierbarer Dehnungssensoren werden international untersucht. Die Verringerung des Sensordurchmessers auf Abmaße im Bereich des Durchmessers von Verstärkungsfasern ist dabei ein bedeutendes Entwicklungsziel. Insbesondere bei der Integration in Bauteile aus faserverstärkten Kunststoffen sorgen zum Durchmesser von Fasern vergleichbare Sensordurchmesser für eine optimale Sensoranbindung. Die Bildung von Harznestern sowie schwächender Unstetigkeiten kann mittels dünner Sensoren verhindert werden. Dies gewährleistet eine artefaktefreie Dehnungsmessung. Drei verschiedene Ansätze für neuartige Dehnungssensoren mit kleinem Querschnitt wurden in dieser Arbeit untersucht. / Strain sensors are used for structural health monitoring issues, certainly in parts with high safety requirements made of fibre-reinforced plastic composites. The integration of these sensors inside the parts protects them against any mechanical and corrosive impact. The sensor functionality can be enhanced by integration. There is a lot of international research effort to further develop integratable strain sensors. Different approaches are currently pursued. This thesis presents the results of investigations on three different approaches for novel strain sensors. The main goal of these investigations was to minimise the sensor diameter down to the diameter of reinforcing fibres. The small diameter allows for an optimum and artefact free integration of the sensors. The formation of resin nests and notches to the material structure can be prevented by integrating sensor with a smaller diameter. The strain measurement and monitoring is enhanced and more reliable then.