Influence of substrate temperature on the microstructure of YSZ films and their application as the insulating layer of thin film sensors for harsh temperature environments

Thin film sensors are employed to monitor the health of hot-section components of aeroengine intelligence (for instance, blades), and electrical insulating layers are needed between the metal components and thin film sensors. For this purpose, the electrical insulation characteristics of an yttria-stabilized zirconia (YSZ)/Al₂O₃ multilayer insulating structure were investigated. First, YSZ thin films were deposited by DC reactive sputtering at various substrate temperatures, and the microstructural features were investigated by scanning electron microscopy and X-ray diffraction. The results indicate that the micromorphology of the YSZ thin film gradually became denser with increasing substrate temperature, and no new phases appeared. The compact and uniform topography of the YSZ thin film improved the insulation properties of the multilayer insulating structure and enhanced the adhesion of the thin film sensors. In addition, the electrical insulation properties of the YSZ/Al₂O₃ multilayer insulating structure were evaluated via insulation resistance tests from 25 to 800 °C, in which the YSZ thin film was deposited at 550 °C. The results show that the insulation resistance of the multilayer structure increased by an order of magnitude compared with that of the conventional Al₂O₃ insulating layer, reaching 135 kΩ (5.1 × 10^?6 S/m) at 800 °C. Notably, the insulation resistance was still greater than 75 kΩ after annealing at 800 °C for 5 h. Finally, the shunt effect of the YSZ/Al₂O₃ multilayer insulating structure was estimated using a PdCr thin film strain gauge. The relative resistance error was 0.24%, which demonstrates that the YSZ/Al₂O₃ multilayer insulating structure is suitable for thin film sensors.     

Orientation control and electrical properties of PZT/LNO capacitor through chemical solution deposition

This paper describes the deposition of PZT/lanthanum nickel oxide (LNO) electrode thin-film capacitor on a Si(1 0 0) substrate with a chemical solution deposition (CSD). Highly (1 0 0)-oriented LNO film with a perovskite structure was deposited by annealing at 700 °C from a precursor solution of La(NO₃)₃ and Ni(CH₃COO)₂. In addition, highly (1 0 0)&(0 0 1)-oriented PZT/LNO capacitor was deposited on LNO/Si substrate by annealing at 600 °C, showing P_r = 18 μC/cm² and E_c = 36 kV/cm. Furthermore, the resultant PZT/LNO thin-film capacitor exhibited no fatigue up to 10⁸ switching cycles.     

Rapid Microwave Annealing of Amorphous Lead Zirconate Titanate Thin Films Deposited by Sol‐Gel Method on LaNiO3/SiO2/Si Substrates

The heating behavior of LaNiO₃ (LNO) films on SiO₂/Si substrate heated by 2.45 GHz microwave irradiation in the microwave magnetic field was first investigated, and then amorphous Pb(Zr_0.52Ti_0.48)O₃ (PZT) thin films were deposited on LNO‐coated SiO₂/Si substrates by a sol‐gel method and crystallized in the microwave magnetic field. The crystalline phases and microstructures as well as the electrical properties of the PZT films were investigated as a function of the elevated temperature generated by microwave irradiation. The perovskite PZT films with a highly (100)‐preferred orientation can be obtained by microwave annealing at 700°C for only 180 s of total processing time, and have good electrical properties. The results demonstrated that conductive metal oxide LNO as a bottom electrode layer is an advantage for the crystallization of PZT thin films by microwave irradiation in the microwave magnetic field.     

Wide Color Variation in SiNO Thin Films Dispersed with Precipitated TiN Nano Particles

Amorphous thin films of Ti_1?ySi_y(N,O) with y ≥ 0.38 were prepared by reactive sputter deposition in a nitrogen atmosphere. Thermal annealing of the films in an ammonia flow above 800°C yielded Si(N,O) amorphous thin films dispersed with precipitated TiN nanosized particles. The film color changed with Si content y and the annealing conditions, from carrot orange to cream yellow in the as‐deposited films due to their oxynitride nature, and from dark green to canary yellow and from iron blue to horizon blue at respective annealing temperatures of 800°C and 900°C due to metallic nature of the TiN nanosized particles precipitated in the annealing.     

Seed layer mediated growth of high dielectric and low leakage BaTiO3 thin film using two-step sputtering process

In this study, we demonstrated the seed layer mediated growth of high-quality BaTiO₃ (BTO) thin films using a two-step radio frequency (RF) magnetron sputtering process. Since the as-grown BTO thin films obtained by RF magnetron sputtering at the deposition temperatures of 300–500 °C were amorphous with a low dielectric constant of 20, it is necessary to develop a fabrication process for obtaining crystalline high-k BTO thin films without sacrificing other film properties such as morphology and leakage current. First, it was revealed that ex-situ post-deposition annealing (PDA) at high temperatures in the 700–800 °C range led to the crystallization of BTO films and a high dielectric constant of 121. However, the film morphology deteriorated significantly during PDA, and consequently, a high leakage current was observed due to the rough and discontinuous surface containing voids and micro-cracks. To achieve an excellent leakage current characteristic as well as a high dielectric constant for a crystalline BTO thin film, in-situ crystallization was carried out through local epitaxial growth using a crystalline seed layer. The crystalline BTO seed layer was formed by annealing a 5-nm-thick amorphous BTO film at 700 °C on which the in-situ crystallized BTO main layer was deposited at 500 °C. The in-situ crystallization method resulted in a smooth and uniform surface and a high dielectric constant of 113. In addition, the in-situ crystallized BTO film exhibited a low leakage current density of 10⁻⁶ A/cm² (at 0.8 V) displaying an improvement by a factor of 10³ compared to the ex-situ crystallized BTO film.     

Deposition of highly oriented lanthanum nickel oxide thin film on silicon wafer by CSD

This paper describes the orientation control and the electrical properties of the chemical solution deposition (CSD) derived LaNiO₃ (LNO) thin film. The LNO precursor solutions were prepared using lanthanum nitrate and nickel acetate as La and Ni source, and ethanol or 2-methoxyethanol and 2-aminoethanol mixed solution as solvents. The LNO films were spin-coated using these precursor solutions and annealed at the temperature from 500 to 700 °C. The resulting LNO film annealed at 700 °C derived from 2-methoxyethanol and 2-aminoethanol mixed solvent exhibited (1 0 0)-orientation, with some surface cracks and pores, and relatively higher resistivity of 2.49 × 10⁻³ Ω cm. The LNO film derived from 2-methoxyethanol and 2-aminoethanol mixed solvent annealed at 700 °C in an oxygen atmosphere showed highly (1 0 0)-orientation, with higher density, a few cracks and pores, and exhibited a good electrical resistivity of 7.27 × 10⁻⁴ Ω cm.     

Annealing temperature-dependent structural and electrical properties of (Ta2O5)1-x - (TiO2)x thin films,x ≤ 0.11

(Ta₂O₅)_1-x- (TiO₂)_x (TTO_x) thin films, with x = 0, 0.03, 0.06, 0.08, and 0.11, were deposited using magnetron direct current (DC) sputtering method onto the P/boron-silicon (1 0 0) substrates by varying areas of Tantalum and Titanium metallic targets, in oxygen environment at ambient temperature. The as-deposited thin films were annealed at temperatures ranging from 500 to 800 °C. Generally, the formation of the Ta₂O₅ structure was observed from the X-ray diffraction measurements of the annealed films. The capacitance of prepared metal– oxide– semiconductor (MOS) structures of Ag/TTO_x/p-Si was measured at 1 MHz. The dielectric constant of the deposited films was observed altering with varying composition and annealing temperature, showing the highest value 71, at 1 MHz, for the TTO_x films, x = 0.06, annealed at 700 °C. With increasing annealing temperature, from 700 to 800 °C, the leakage current density was observed, generally decreasing, from 10^?5 to 10^?8 A cm^?2, for the prepared compositions. Among the prepared compositions, films with x = 0.06, annealed at 800 °C, having the observed value of dielectric constant 48, at 1 MHz; and the leakage current density 2.7 × 10^?8 A cm^?2, at the electric field of 3.5 × 10⁵ V cm^?1, show preferred potential as a dielectric for high-density silicon memory devices.     

Effect of silver content on the microstructure,thermal stability and mechanical properties of CrNx/Ag nanocomposite films

CrN_x/Ag nanocomposite films with varying Ag content were prepared by reactive magnetron sputtering under a constant Ar/N₂ stream. The films were annealed between 500 – 800 °C in the air. The microstructure and elemental composition of films were studied by X-ray diffraction, scanning electron microscopy and energy dispersive spectroscopy. The mechanical properties were characterized with respect to nano-hardness and high-temperature tribology. The results reveal that the incorporation and concentration of Ag influence the morphology and microstructure of films. The microstructure of films evolves by annealing, and the films with higher Ag concentration exhibit more severe structure evolution. Annealing at 650 °C results in the sublimation of Ag, and the oxide emerges on the film surface. Annealing at 800 °C reveals that the film with 6.2 at.% Ag exhibits superior structural stability, while the one with 20.2 at.% Ag deteriorates. The hardness of films decreases with the increasing Ag concentration and heating temperature. Films with 12.6 at.% Ag and above possess solid lubrication during the sliding at 350–650 °C. Both the friction coefficient and wear resistance are found dependent on the Ag concentration and sliding temperature.     

Thermal stability of MgO film on Si grown by atomic layer deposition using Mg(EtCp)2 and H2O

MgO films were deposited on Si via atomic layer deposition (ALD) using Mg(EtCp)₂ and H₂O precursors and their thermal stability was examined as a function of the post-deposition annealing (PDA) temperature. The characteristic self-limiting behavior of the ALD process was confirmed by changing several parameters, such as precursor pulsing times, deposition temperature, and number of cycles. The exceptional resulting step coverage was verified on a patterned wafer with a high aspect ratio. The band gap and dielectric constant of the as-deposited ALD-MgO film were extracted to be approximately 7.5 eV and 8.4, respectively, and were stable up to the PDA temperature of 700 °C. However, considerable outward diffusion of the underlying Si atoms toward MgO started to occur above 700 °C, and most of the MgO film was converted to an amorphous Mg-silicate phase at 900 °C with a thin layer of remaining MgO on top.     

Highly ordered columnar ITO thin film with enhanced thermoelectric and mechanical performance over wide temperature range

Indium tin oxide (ITO) based thin films offer the possibility to improve the performance of high-temperature thermocouples by providing good sensitivity and reliability over a wide temperature range. In this study, a thin but robust ITO-based thin-film thermocouple, with a low-crystallised highly ordered columnar structure, was fabricated. The electrical conductivity exhibited a high temperature-dependent sensitivity owing to the increasing density with increasing temperature. The nano-hardness and interfacial robustness were evaluated and found to exhibit excellent service reliability at high temperatures because of the low thermal stress. Furthermore, the similar mechanical and electrical performances of the thin films, after annealing at 600 and 800 °C, demonstrated that the enhanced performance was mainly determined by the orientation of the ITO thin films. An enhanced Seebeck coefficient (～100 μV K^?1) was obtained for the ITO thin film after annealing at 1000 °C, resulting in a special structure with profuse nanoholes. These results highlight the good mechanical performance and stability of the thermoelectric properties of highly ordered columnar thin films over a wide temperature range, and can serve as a guide for the preparation of thin but robust functional ceramic-based materials.     

Low-temperature crystallization of tantalum pentoxide films under elevated pressure

Ta₂O₅ thin films deposited via a metal-organic decomposition method were crystallized via atmospheric pressure annealing and a high-pressure crystallization (HPC) process. Ta₂O₅ thin films started to become crystallized at 700 °C as subjected to atmospheric pressure annealing. When the HPC process was adopted and annealing at 16.5 MPa was performed, the crystallization temperature of Ta₂O₅ films was greatly dropped to as low as 350 °C. The developed HPC process considerably reduced the thermal budget and energy consumption during film processing. The crystallized Ta₂O₅ phase was found to be homogeneously distributed within the HPC-derived films. With annealing at 700 °C under atmospheric pressure, the silicon species diffused from the substrates into the Ta₂O₅ layers, thereby leading to reduced dielectric constants. The HPC process effectively suppressed the interdiffusion between the substrates and dielectric layers by lowering the required heating temperature, and also significantly increased the dielectric constants of Ta₂O₅ thin films. The HPC process was confirmed to effectively lower the crystallization temperature and improve the dielectric properties of Ta₂O₅ thin films.     

Fabrication and Dielectric Properties of Ba0.63Sr0.37TiO3 Thin Films on SiC Substrates

Ba_0.63Sr_0.37TiO₃ (BST) films were first deposited on SiC substrates with LNO bottom electrodes by magnetron sputtering. The BST/LNO/SiC thin films exhibit high dielectric tunability and low dielectric loss while maintaining excellent temperature coefficient of dielectric constant in the temperature range between 250 and 350 K. We also investigated the effect of film thickness on the dielectric properties. BST(430 nm)/LNO/SiC film has higher tunability (68.09% @700 kV/cm), lower loss tangent (tanδ = 0.00987) and quite a bit higher figure of merit (FOM = 68.99) as compared with that of BST(300 nm)/LNO/SiC film. Our results demonstrate that combining ferroelectric BST films with SiC substrates is very promising for the development of tunable devices over a large temperature range.     

The effects of deposition temperature on structure and dielectric properties of Ba0.6Sr0.4TiO3 thin films produced by pulsed laser deposition

The effects of deposition temperature on orientation, surface morphology and dielectric properties of the thin films for Ba_0.6Sr_0.4TiO₃ thin films deposited on Pt/Ti/SiO₂/Si substrates by pulsed laser deposition were investigated. X-ray diffraction patterns revealed a (2 1 0) preferred orientation for all the films. With rising substrate temperature from 650 °C to 700 °C, the crystallinity and crystal grain size of the films increase, the relative dielectric constant increases, but the dielectric losses have not obvious difference. The film deposited at 350 °C and annealed at 700 °C has strongly improved roughness and dielectric permittivity compared with the film only deposited directly at 700 °C. Three distinct relaxation processes within tan(δ) were found for the Ba_xSr_1?xTiO₃ film: a broadened process of the film relaxation, an intermediate peak which originates from Maxwell–Wagner–Sillars polarization, and an extremely slow process ascribed to leak current. The complex dielectric permittivity and loss can be fitted by an improved Cole–Cole model corresponding to a stretched relaxation function.     

Low‐Temperature Deposition of Hexagonal Boron Nitride via Sequential Injection of Triethylboron and N2/H2 Plasma

Hexagonal boron nitride (hBN) thin films were deposited on silicon and quartz substrates using sequential exposures of triethylboron and N₂/H₂ plasma in a hollow‐cathode plasma‐assisted atomic layer deposition reactor at low temperatures (≤450°C). A non‐saturating film deposition rate was observed for substrate temperatures above 250°C. BN films were characterized for their chemical composition, crystallinity, surface morphology, and optical properties. X‐ray photoelectron spectroscopy (XPS) depicted the peaks of boron, nitrogen, carbon, and oxygen at the film surface. B 1s and N 1s high‐resolution XPS spectra confirmed the presence of BN with peaks located at 190.8 and 398.3 eV, respectively. As deposited films were polycrystalline, single‐phase hBN irrespective of the deposition temperature. Absorption spectra exhibited an optical band edge at ~5.25 eV and an optical transmittance greater than 90% in the visible region of the spectrum. Refractive index of the hBN film deposited at 450°C was 1.60 at 550 nm, which increased to 1.64 after postdeposition annealing at 800°C for 30 min. These results represent the first demonstration of hBN deposition using low‐temperature hollow‐cathode plasma‐assisted sequential deposition technique.     

Temperature and processing effects on lithium ion conductivity of solution-deposited lithium zirconium phosphate (LiZr2P3O12) thin films

Lithium zirconium phosphate (LiZr₂P₃O₁₂) thin films have been prepared on platinized silicon substrates via a chemical solution deposition approach with processing temperatures between 700°C and 775°C. Films that were subject to a single high-temperature anneal were found to crystallize at temperatures above 725°C. Crystallization was observed in films annealed after each deposited layer at 700°C and above. In both cases, grain size was found to increase with annealing temperature. Ion conductivity was found to increase with annealing temperature in singly annealed films. In per-layer annealed films ion conductivity was found to initially increase then decrease with increasing annealing temperature. A maximum ion conductivity of 1.6 × 10⁻⁶ S/cm was observed for the singly annealed 775°C condition, while a maximum ion conductivity of 5.8 × 10⁻⁷ S/cm was observed for the 725°C per-layer annealed condition. These results are consistent with an increasing influence of cross-plane, internal interface resistance and vapor phase carrier loss in the per-layer annealed samples. This work demonstrates that post-deposition processing methods can strongly affect the ion conducting properties of LiZr₂P₃O₁₂ thin films.     

High temperature lattice structure evolution of C-axis preferred orientation AlN thin films and its application in temperature measurement

In order to measure the surface temperature of aerospace hot-end components accurately, AlN thin film temperature measurement technology was explored. In this research, C-axis preferred orientation AlN thin film was deposited on Ni-based superalloy substrates by medium frequency (MF) reaction magnetron sputtering. Effect of temperature on the lattice structure of AlN thin film was studied. X-ray diffraction results show that the diffraction angles (2θ) of AlN thin films shift to the left side monotonously with the increase of annealing temperature and annealing time. Based on this phenomenon, the maximum temperature experienced by the film can be deduced according to 2θ values. A temperature interpretation algorithm equation was established with MATLAB. The algorithm is a binary linear equation, whose dependent variable is 2θ and the independent variables are annealing temperature and annealing time. Then, temperature interpretation software was developed with Visual Studio 2019. The temperature interpretation range is 700–1200 °C and the relative interpretation error is less than 4.26%.     

Effect of annealing temperature on ferroelectric electron emission of sol–gel PZT films

In this work, the influence of annealing temperature on the ferroelectric electron emission behaviors of 1.3-μm-thick sol–gel PbZr_0.52Ti_0.48O₃ (PZT) thin film emitters was investigated. The results revealed that the PZT films were crack-free in perovskite structure with columnar-like grains. Increasing annealing temperature led to the growth of the grains with improved ferroelectric and dielectric properties. The remnant polarization increased slightly from 35.3 to 39.6 μC/cm² and the coercive field decreased from the 56.4 to 54.6 kV/cm with increasing annealing temperature from 600 to 700 °C. The PZT film emitters exhibited remarkable ferroelectric electron emission behaviors at the threshold voltage above 95 V. The film annealed at 700 °C showed a relatively lower threshold voltage and higher emission current, which is related to the improved ferroelectric and dielectric properties at higher annealing temperature. The highest emission current achieved in this work was around 25 mA at the trigger voltage of 160 V.     

Thermal stability and mechanical properties of HVOF/PVD duplex ceramic coatings produced by HVOF and cathodic vacuum arc

Duplex ceramic coatings, consisting of an inner NiCr-Cr₃C₂-based coating and an outmost AlCrN film, were produced on the steel substrate in succession by velocity oxygen-fuel spraying (HVOF) and cathodic vacuum arc methods, and then isochronally annealed at annealing temperatures below 900 °C for 2 h. The thermal stability and mechanical properties of the annealed samples were systematically studied by means of X-ray diffraction, Optical microscope and transmission electron microscope, in association with mechanical property measurements. The results show that the microstructure, phase evolution and mechanical properties of duplex ceramic coatings are significantly dependent on the annealing temperature. Metastable fcc-AlCrN solid solution in AlCrN film first decomposes to rich-Al and rich-Cr domains by spinodal decomposition at 700 °C, leading to a notable increase in hardness due to its smaller grain size and high elastic strain field, and then to equiaxed hcp-AlN and Cr₂N by the nucleation and growth at 900 °C, leading to a notable decrease in hardness due to the recrystallization and the formation of hcp-AlN. Meanwhile, the both decarburization of Cr₃C₂ to Cr₇C₃ occurs at 800 °C, but becomes more intensive at 900 °C, leading to a notable loss in hardness. In addition, the dissolution of Cr₃C₂ produces high density of porosity, which also reduces the hardness. The hardness tests show the following ordering of load-bearing capacity for the duplex ceramic coatings: 700 °C>As-deposited >800 °C>900 °C. Tribological property measurements demonstrate that the wear resistance of the tested duplex ceramic coatings obeys the following ordering: 700 °C>As-deposited >800 °C>900 °C. The improved wear resistance is due to high surface hardness, load-bearing capacity and thermal stability. In addition, the wear mechanisms are shown.     

Temperature-independent physical properties of electrophoretic Ti5NbO14 films for high-temperature capacitors

Ti₅NbO₁₄ (T5NO) films were developed on Pt/Ti/SiO₂/Si substrates by electrophoretic method by using T5NO³⁻ nanosheets. The film deposited at room temperature (RT) contained organic defects, which were almost eliminated in the film annealed at 700 °C. The film deposited at RT revealed (100) planes with an inter-planar distance of 1.1 nm because of the existence of TBA⁺ defects. However, for the films annealed at higher temperatures (≥400 °C), two types of structures formed: (100) planes with 0.55 nm inter-planar distance (group-1 structure), and (100) planes with 1.42 nm inter-planar distance (group-2 structure). The dielectric constant (ε_r) of the film annealed at 700 °C was 61 with a low dielectric loss of 1.0%. Variations in the ε_r according to the film thickness, electric field, and temperature were small. This film displayed a high insulating property up to 300 °C with a small temperature coefficient of capacitance (−56.7 ppm/K) up to 400 °C.     

Electrochemical performance of La2NiO4+δ cathode for intermediate-temperature solid oxide fuel cells

The application of the La₂NiO_4+δ (LNO), one of the Ruddlesden–Popper series materials, as a cathode material for intermediate temperature solid oxide fuel cells is investigated in detail. LNO is synthesized via a complex method using ethylenediaminetetraacetic acid (EDTA) and citric acid. The effect of the calcination temperature of the LNO powder and the sintering temperature of the LNO cathode layer on the anode-supported cell, Ni–YSZ/YSZ/GDC/LNO, is characterized in view of the charge transfer resistance and the mass transfer resistance. Charge transfer resistance was not significantly affected by calcination and sintering temperature when the sintering temperature was not lower than the calcination temperature. Mass transfer resistance was primarily governed by the sintering temperature. The unit cell with the LNO cathode sintered at 1100 °C with 900 °C-calcined powder presented the lowest polarization resistance for all the measured temperatures and exhibited the highest fuel cell performances, with values of 1.25, 0.815, 0.485, and 0.263 W cm⁻² for temperatures of 800, 750, 700, and 650 °C, respectively.