The lithium tantalite [LiTaO3,abbreviated to LT] thin films were deposited on Pt/SiO2/Si substrates by spin coating with sol-gel processing and rapid thermal processing in this thesis. 1,3 propanediol was used as solvent to minimize the number of cycles of spin coating and drying processes to obtain the desired thickness of thin film. By changing the heating rate (600~3000¢J/min) and the heating temperature (500~800¢J), the effects of various processing parameters on the thin films growth are studied. The effects of various heating rate on the response of pyroelectric IR detector devices are studied also. Experimental results reveal that the heating rate will influence strongly on grain size, dielectricity, ferroelectricity and pyroelectricity of LT thin films. With the increase of heating rate, the grain size of LT thin film decreases slightly, and the C-axis orientation is enhanced. The relative dielectric constant of LT thin film increases from 28 up to 45.6, the tand increases from 0.033 to 0.134, Ec increases from 122 KV/cm to 183 KV/cm, Pr increases from 7.45 mC/cm2 to 12.12 mC/cm2, and g increases from 9.33´10-9 C/cm2K up to 2.66´10-8 C/cm2K, respectively, as the heating rate increases form 600 up to 3000¢J/min. In addition, the results also show that the LT thin film possesses the largest figures of merit Fv (2.19¡Ñ10-10 Ccm/J) and Fm (4.01¡Ñ10-9 Ccm/J) at the heating temperature of 700¢J and heating rate of 1800¢J/min. The voltage responsivities (Rv) measured at 80 Hz increase from 5496 to 8455 V/W and the specific detecivities (D*) measured at 300 Hz increase from 1.94¡Ñ108 to 2.38¡Ñ108 cmHz1/2/W with an increase of heating rate from 600 to 1800¢J/min. However, the voltage responsivity and the specific detecivity decrease with heating rate in excess of 1800¢J/min. The results show that LT1800 pyroelectric thin film detector exists both the maximums of voltage responsivity and specific detecivity. Therefore, LT1800 thin film exhibits the best IR characteristics for detector material.

In this thesis, the lithium tantalite [LiTaO3, abbreviated to LT] thin films were deposited on Pt/Ti/SiO2/Si substrates by spin coating with sol-gel processing and rapid thermal processing. 1,3 propanediol was used as solvent to minimize the number of cycles of spin coating and drying processes to obtain the desired thickness of thin film. By changing the heating rate (600~3000¢J/min) and the heating temperature (500~800¢J), the effects of various processing parameters on the thin films growth are studied. In addition, the thermal isolation of detecting elements was achieved by the anisotropic wet etching of back silicon substrate. In order to reduce the thermal mass and thermal time constant of detector, the sensing element was built-up on a thin membrane. By changing the membrane thickness (20~350 £gm), the effects of various membrane thickness on the response of pyroelectric IR detector devices are studied also. Experimental results reveal that the heating rate will influence strongly on grain size, dielectricity, ferroelectricity and pyroelectricity of LT thin films. With the increase of heating rate, the grain size of LT thin film decreases slightly, and the c-axis orientation is enhanced. The relative dielectric constant (£`r ) of LT thin film increases from 28 up to 45.6, the dielectric loss (tan

Les matériaux ferroélectriques sont caractérisés par l'existence d'une polarisation électrique spontanée, dont l'orientation peut être inversée par l'application d'un champ électrique adéquat. Permettant de coder l'information sous la forme d'un domaine ferroélectrique, i.e. une région du matériau avec une certaine orientation de la polarisation, les ferroélectriques ouvrent la voie au stockage de masse de très haute densité (>10 Tbit/in ²). Dans ce contexte, nous avons employé la Piezoresponse Force Microscopy (PFM), un mode particulier de Microscope à Force Atomique (AFM), permettant la manipulation et la détection des domaines ferroélectriques à l'échelle du nanomètre. Avec pour objectif d'étudier les mécanismes de formation des domaines par l'intermédiaire d'une pointe AFM, nos travaux ont mis en valeur la cinétique de croissance des domaines dans des films minces monocristallins de LiTaO3, avec une approche complémentaire de celle thermodynamique, dépendante du champ électrique et soulignant le rôle de l'humidité dans une possible conduction de surface. En parallèle, les films de LiTaO3 ont permis d'appréhender davantage la nature électro-mécanique de la réponse PFM, pour notamment relier l'amplitude du signal mesuré à la géométrie du domaine sous pointe. PFM et domaines ferroélectriques se sont en effet révélés tour à tour, objet d'étude et outil de caractérisation.

Optical parametric frequency conversion based on quasi phase matching (QPM) in nonlinear optical crystals is a powerful technique for generating coherent radiation in wavelength ranges spanning from the mid-infrared (mid-IR) to the blue, displaying low thermal load and high efficiency.This thesis shows how QPM in one- (1D) or two-dimensional (2D) lattices can be employed to engineer novel devices for parametric downconversion in the IR, af-fording freedom in designing both spectral and angular properties of the parametric output. Experimental demonstrations of parametric devices are supported by theoreti-cal modelling of the nonlinear conversion processes.In particular, broadband parametric downconversion has been investigated in 1D QPM lattices, through degenerate downconversion close to the point of zero group-velocity dispersion. Ultra-broadband optical parametric generation (OPG) of 185 THz bandwidth (at 10 dB), spanning more than one octave from 1.1 to 3.7 μm, has been achieved in periodically poled 1 mol% MgO-doped near-stoichiometric LiTaO3 (MgSLT) of 25 μm QPM period, pumped at 860 nm. Such broadband gain is of high interest for ultrashort optical pulse amplification, with applications in high harmonic generation, ultrafast spectroscopy and laser ablation. Furthermore, the det-rimental impact of parasitic upconversion, creating dips in the OPG spectrum, has been investigated. By altering the pump pulse duration, energy can be backconverted to create peaks at the involved OPG wavelengths, offering a possible tool to enhance broadband parametric gain spectra.The engineering of the angular properties of a parametric output benefits greatly from 2D QPM, which is investigated in this thesis by the specific example of hexagonally poled MgSLT. It is demonstrated how two OPG processes, supported by a single 2D QPM device, can exhibit angularly and spectrally degenerate signals (idlers). This degeneracy results in a coherent coupling between the two OPG pro-cesses and a spectrally degenerate twin-beam output in the mid-IR (near IR). 2D QPM devices exhibiting such coherently coupled downconversion processes can find applications as compact sources of entangled photon-pairs. This thesis further illus-trates the design freedom of 2D QPM through the demonstration of a device support-ing multiple parametric processes, thus generating multiple beams from the mid-IR to the blue spectral regions. / <p>QC 20131204</p>

Nonlinear optical frequency conversion is one of the most important key techniques in order to obtain lasers with wavelengths targeted for specific applications. In order to realize efficient and tailored lasers, the quasi-phase-matching (QPM) approach using periodically-poled ferroelectric crystals is getting increasingly important. Also understanding of damage mechanisms in nonlinear materials is necessary to be able to design reliable and well working lasers. This is especially true for high power application lasers, which is a rapidly growing field, where the damage problem normally is the ultimate limiting factor. In this thesis work, several promising novel ferroelectric materials have been investigated for nonlinear optical applications and the emphasis has been put on QPM devices consisting of periodically-poled structures. The materials were selected from three different types of ferroelectric materials: 1) MgO-doped stoichiometric LiNbO3 (MgO:SLN) and LiTaO3 (MgO:SLT), and non-doped stoichiometric LiTaO3 (SLT), 2) KTiOPO4 (KTP) and its isomorphs RbTiOPO4 (RTP), and 3) KNbO3 (KN). The focus in our investigations have been put on the spontaneous polarization switching phenomena, optimization of the periodic poling conditions, and the photochromic optical damage properties which were characterized by the help of blue light-induced infrared absorption (BLIIRA) measurements. With electrical studies of the spontaneous polarization switching, we were able to determine quantitatively, and compare, the coercive field values of different materials by applying triangularly shaped electric fields. We found that the values of the coercive fields depended on the increase rate of the applied electric field. The coercive field of KN was the lowest (less than 0.5 kV/mm) followed by the ones of KTP, SLT, and MgO:SLT (1.5 to 2.5 kV/mm). MgO:SLN, and RTP had relatively high coercive fields, approximately 5.0 to 6.0 kV/mm, respectively. Based on the domain switching characteristics we found, we successfully fabricated periodically-poled devices in all of the investigated materials with 30 μm periodicities and sample thickness of 1 mm. Blue light-induced infrared absorption (BLIIRA) has been characterized for unpoled bulk and periodically-poled samples using a high-sensitivity, thermal-lens spectroscopy technique. SLT showed a large photorefraction effect and the BLIIRA signal could not be properly measured because of the large distortion of the probe beam. The rise and relaxation time of BLIIRA, after switching the blue light on and off was in a time span of 10 to 30 sec except for KTP and its isomorphs, which needed minutes to hours in order to saturate at a fixed value. KN and MgO:SLN showed the lowest susceptibility to the induced absorption. Periodic poling slightly increased the susceptibility of KTP, MgO:SLT, and KN. Relatively high thresholds were observed in MgO:SLT and KN. By increasing the peak-power intensity of the blue light, the induced absorption for MgO:SLN, KTP and KN saturated at a constant value while that of MgO:SLT increase in a constant fashion. This trend is critical issue for the device reliability at high-power applications. / QC 20100830

Les matériaux ferroélectriques sont caractérisés par l'existence d'une polarisation électrique spontanée, dont l'orientation peut être inversée par l'application d'un champ électrique adéquat. Permettant de coder l'information sous la forme d'un domaine ferroélectrique, i.e. une région du matériau avec une certaine orientation de la polarisation, les ferroélectriques ouvrent la voie au stockage de masse de très haute densité (>10 Tbit/in ²). Dans ce contexte, nous avons employé la Piezoresponse Force Microscopy (PFM), un mode particulier de Microscope à Force Atomique (AFM), permettant la manipulation et la détection des domaines ferroélectriques à l'échelle du nanomètre. Avec pour objectif d'étudier les mécanismes de formation des domaines par l'intermédiaire d'une pointe AFM, nos travaux ont mis en valeur la cinétique de croissance des domaines dans des films minces monocristallins de LiTaO3, avec une approche complémentaire de celle thermodynamique, dépendante du champ électrique et soulignant le rôle de l'humidité dans une possible conduction de surface. En parallèle, les films de LiTaO3 ont permis d'appréhender davantage la nature électro-mécanique de la réponse PFM, pour notamment relier l'amplitude du signal mesuré à la géométrie du domaine sous pointe. PFM et domaines ferroélectriques se sont en effet révélés tour à tour, objet d'étude et outil de caractérisation. / Ferroelectric materials are characterized by their spontaneous polarization, whose direction can be reversed by the application of a suitable electric field. Using domains, i.e. regions of uniform polarization orientation, as information bits, ferroelectrics opens the pathway towards ultrahigh storage densities (>10 Tbit/in²). In this respect, Piezoresponse Force Microscopy (PFM), a technique derived from Atomic Force Microscopy (AFM), was used to manipulate and detect ferroelectric domains on the nanometer scale. Our study was focused on the domains formation mechanism in the local electric field of a nanosized tip. Within an approach complementary to the thermodynamic one, we underlined the kinetics of domains growth in single-crystal LiTaO3 thin films, and the role of humidity in a possible surface conduction. In parallel, the LiTaO3 thin films were used to better understand the PFM response, in particular the relation between the measured signal and the geometry of the domain below the tip. This way, PFM and ferroelectrics domains alternately appeared as object of study and characterization tool.

In this thesis, the results pertaining to various investigations carried out on Triglycine sulphate (TGS) single crystals, polyvinylidene fluoride (PVDF) films, lithium tantalate (LT)/PVDF nanocomposites and LT thin films are presented with emphasis on the characteristics that are crucial for their use in pyroelectric sensors. TGS single crystals (size 68 x 45 x 42 mm3), which have high pyroelectric coefficients, were grown by slow cooling method using newly designed platform technique based crystal growth work stations. The problem of slow growth rate along c-direction was overcome by placing (010) oriented seeds on the platform. The grown TGS crystals were used for the fabrication of the laser energy meter and temperature sensor. One drawback of TGS is its low Curie temperature (490C). As a consequence when the operating temperature approaches the Curie temperature, the crystals start depolarizing owing to the movement of domains. As a result the linearity of the devices gets affected and restricts the use of TGS. Therefore pyroelectric materials possessing higher Curie temperatures and larger pyroelectric coefficients than that of TGS are desirable. LT in single crystalline form having Curie temperature of ≈6000C has already been in use for pyroelectric device applications. However, growing stoichiometric LT single crystal is very difficult. On the other hand PVDF polymer films (Tc≈1800C) have low pyrolectric coefficients and difficult to pole electrically. Therefore efforts were made to prepare LT/PVDF nanocrystal composites to increase the pyroelectric coefficient of PVDF and to reduce the poling field. Nanoparticles of LT were prepared using sol-gel route. Spherical nanoparticles of size 20-40nm were prepared from sol by adding oleic acid to it. These nanoparticles were characterized using XRD, TEM, DSC and Raman spectroscopy. PVDF films with large percentage of β-phase (ferroelectric phase) were fabricated from solutions prepared using dimethylsulphoxide (DMSO) solvent. PVDF films (30µm thick), embedded with 20-40nm sized nanocrystallites of LT were fabricated to utilize them for pyroelectric sensor applications. The ferroelectric and pyrolectric properties of nano composite films were studied for sensor applications point of view. As a replacement for the single crystals of LT in pyroelectric sensors, investigations were carried out on oriented LT thin films. The studies on LT thin films yielded promising results which could be exploited for pyroelectric sensor applications.

The ability of physics to provide an understanding of our Universe lies in the essential interrelation between experiment and theory. But physics does not provide us only reliable representations of the causes acting in nature. Its powerful experimental devices and theoretical methods are the underlying reason of the explosive technological development of our time. LiNbO3 and LiTaO3 represent only one example of the essential impact of both experimental and theoretical investigations on their technological applications. Particularly, LiNbO3 has been the subject of many experimental studies due to its applications in electro-optic and integrated optical devices. Also, the doped LiNbO3 with rare-earth and transition metals could be used, for instance, as a material for tunable lasers. The previous theoretical studies devoted to LiNbO3 and LiTaO3 focused on their electronic structure, being an attempt to understand the microscopic origin of the paraelectric-to-ferroelectric phase transition of these materials. The ab initio lattice dynamics investigations performed so far were mainly aimed to identify the role of the individual atoms vibrations in the energetic of the phase transition. The lack of a reliable model for the zone-center lattice dynamics in these compounds motivated us to investigate this issue by means of ab initio frozen-phonon calculations. On the background of the obtained phonon frequencies and eigenvectors, we unambiguously identified all zone-center modes for LiNbO3 and the A1 ones for LiTaO3. Due to the above mentioned enlargement of the technological applications of LiNbO3 by doping with various ions, we focused on the analysis of the ground-state properties of this material when doped with Fe and Cr. Even if the theoretical approach used in our calculations is not predictive with respect to the optical properties of the physical systems in study, a certain insight on this problem could be gained from the analysis of the effect of the atomic positions relaxation on the impurities energy levels localized in the optical band gap.