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Recent advances in machine learning capabilities have increased interest in materials research to improve the efficiency of materials discovery and optimization as well as to better understand the underlying phenomena responsible for the observed physical properties. While combinatorial chemistry and compositional engineering is well established in the development of pharmaceutical and chemical products, its use in the field of bulk functional polycrystalline ceramics is far from mature. In this work, a critical review of a high‐throughput powder‐based dispensing system is provided and the challenges involved with the transition from a conventional, human resources intensive workflow to a fully automated process are highlighted. Based on the lead‐free piezoelectric BiFeO3–BaTiO3 binary system, the applicability and robustness of high‐throughput engineering is investigated to increase data point density in phase diagrams, including the composition variations of the resulting materials. This work presents 16 different BiFeO3–BaTiO3 compositions at four different calcination temperatures, both demonstrating the potential of the system. This is coupled to automated crystal structure analysis, which will be used to investigate the role of calcination temperature on the resulting compositions at room temperature. [ABSTRACT FROM AUTHOR]

The influence of uniaxial compressive stress on small-signal relative permittivity and direct piezoelectric coefficient of polycrystalline Li-modified (K0.5Na0.5)NbO3 (0, 2, and 4 mol. % Li) was characterized as a function of temperature from 25 to 450 °C. These data reveal corresponding anomalies in both the dielectric and piezoelectric properties near the well-known structural phase transitions in (KxNa1 − x)NbO3. In particular, increasing stress was found to shift the orthorhombic–tetragonal (T O − T ) and tetragonal–cubic (T C) phase boundaries to higher temperatures, thereby stabilizing the lower symmetry phases. Experimental results also show that stress up to a critical value flattens the piezoelectric response below T O − T , above which a monotonic decrease is observed. In contrast, permittivity is increased below T O − T with increasing stress. These results are used to construct a stress–temperature phase diagram of Li-modified (K0.5Na0.5)NbO3. [ABSTRACT FROM AUTHOR]

Tailoring the electromechanical properties of a material without altering the original composition is an emerging phenomenon for the optimization of functional properties. Post-sintering annealing with varying maximum temperatures, cooling rates, and atmospheres can influence the crystallographic phases, domain structures, conductivity, mechanical properties, and the temperature stability of the electromechanical properties. K1/2Bi1/2TiO3 (KBT) is a high-temperature stable >280 °C A-site complex perovskite piezoelectric and is critical for high-temperature applications. However, the influence of annealing conditions on crystal structure, domain structure, and functional properties is not well-known. This work demonstrates the effect of annealing cooling rate and maximum temperature on the macroscopic electromechanical response as well as the crystal and domain structure. It is shown that the room-temperature state of KBT can be reversibly switched between the ferroelectric and relaxor state, where the slow cooling from 900 °C favors the stabilization of the relaxor state and quenching induces the ferroelectric state. Importantly, the quenched sample showed a stable piezoelectric coefficient up to 368 °C in the depolarization temperature, an increase of 78 °C. The origin of ferroelectric-relaxor state change is proposed to be related to the A-site cation redistribution and the associated change in the crystal structure and domain structure. [ABSTRACT FROM AUTHOR]

The influence of stress on the small‐signal dielectric permittivity and piezoelectric coefficient of polycrystalline lead‐free perovskite 0.92(Na1/2K1/2)NbO3–(0.08 − x)Bi1/2Li1/2TiO3–xBaZrO3 (x = 0, 0.02, 0.04, 0.06, and 0.07) was characterized under different constant uniaxial stress up to −200 MPa within a temperature range of −150 to 450°C, revealing stress‐induced suppression of the electromechanical response as well as shifts in the phase boundaries. For all compositions, the interferroelectric and ferroelectric–paraelectric phase transitions were shifted to higher temperatures under the uniaxial compressive stress. Interestingly, the sensitivity to the applied stress was found to increase with increasing BZ/BLT ratio in the system. The origin of a different extent of stress‐sensitivity with BZ/BLT ratio is suggested to be related to the change in the crystal structure. Additionally, at temperatures below −50°C, the relative permittivity showed a significant increase under applied compressive stress. [ABSTRACT FROM AUTHOR]

The influence of stress on the phase boundaries of polycrystalline lead-free perovskite (1 − x)Ba(Zr0.2Ti0.8)O3–x(Ba0.7Ca0.3)TiO3 (x = 0.4, 0.5, and 0.6) was characterized through the temperature- and stress-dependent small-signal dielectric and piezoelectric response from − 150 to 200 °C under uniaxial compressive stress up to − 75 MPa. For all three compositions, the phase transition temperatures separating the rhombohedral, orthorhombic, tetragonal, and cubic phases were shifted to higher temperatures with an increase in the uniaxial mechanical loading, corresponding to a significant decrease in the dielectric and piezoelectric responses. Additional stress-dependent relative permittivity measurements up to − 260 MPa were conducted at four different constant temperatures (− 10, 10, 25, and 40 °C), revealing significant increases in the dielectric response, making these materials interesting for tunable dielectric applications. Furthermore, the stress-induced shift in phase transition temperatures was confirmed by in situ combined temperature- and stress-dependent Raman spectroscopy measurements under different constant uniaxial loads within the temperature range from 30 to 130 °C. [ABSTRACT FROM AUTHOR]

Sintering conditions govern the optimized functional properties of ceramics. However, solid-state processing of Bi1/2K1/2TiO3 (BKT), an important end member for lead-free piezoelectric solid solutions suitable for higher temperature (≤ 300 °C) transducer applications, is challenging due to the low melting temperature (≈1070 °C). In this work, the sintering temperature (1030 °C, 1050 °C, and 1060 °C) and dwell time (10 h, 20 h, and 40 h)-dependent functional properties of solid-state processed BKT were investigated, where the sintering condition-dependent dielectric and electromechanical properties were correlated with the variations in crystal structure and microstructure. Although X-ray diffraction data revealed a single-phase tetragonal structure of BKT at room temperature for all sintering conditions, significant changes in both the tetragonal distortion and spontaneous relaxor-ferroelectric transition were observed, which were directly related to the optimized functional properties. In addition, Rayleigh behavior of the piezoelectric coefficient was characterized between −150 °C and 400 °C, demonstrating that the electromechanical response is dominated by the intrinsic contribution, which can be explained by large tetragonal distortion and associated suppression of non-180° domain wall motion. [ABSTRACT FROM AUTHOR]

Sintering conditions govern the optimized functional properties of ceramics. However, solid-state processing of Bi1/2K1/2TiO3 (BKT), an important end member for lead-free piezoelectric solid solutions suitable for higher temperature (≤ 300 °C) transducer applications, is challenging due to the low melting temperature (≈1070 °C). In this work, the sintering temperature (1030 °C, 1050 °C, and 1060 °C) and dwell time (10 h, 20 h, and 40 h)-dependent functional properties of solid-state processed BKT were investigated, where the sintering condition-dependent dielectric and electromechanical properties were correlated with the variations in crystal structure and microstructure. Although X-ray diffraction data revealed a single-phase tetragonal structure of BKT at room temperature for all sintering conditions, significant changes in both the tetragonal distortion and spontaneous relaxor-ferroelectric transition were observed, which were directly related to the optimized functional properties. In addition, Rayleigh behavior of the piezoelectric coefficient was characterized between −150 °C and 400 °C, demonstrating that the electromechanical response is dominated by the intrinsic contribution, which can be explained by large tetragonal distortion and associated suppression of non-180° domain wall motion. [ABSTRACT FROM AUTHOR]

The room temperature aerosol deposition method is especially promising for the rapid deposition of ceramic thick films, making it interesting for functional components in energy, mobility, and telecommunications applications. Despite this, a number of challenges remain, such as an enhanced electrical conductivity and internal residual stresses in as-deposited films. In this work, a novel technique that integrates a sacrificial water-soluble buffer layer was used to fabricate freestanding ceramic thick films, which allows for direct observation of the film without influence of the substrate or prior thermal treatment. Here, the temperature-dependent chemical and structural relaxation phenomena in freestanding BaTiO3 films were directly investigated by characterizing the thermal expansion properties and temperature-dependent crystal structure as a function of oxygen partial pressure, where a clear nonlinear, hysteretic contraction was observed during heating, which is understood to be influenced by lattice defects. As such, aliovalent doping and atmosphere-dependent annealing experiments were used to demonstrate the influence of local chemical redistribution and oxygen vacancies on the thermal expansion, leading to insight into the origin of the high room temperature conductivity of as-deposited films as well as greater insight into the influence of the induced chemical, structural, and microstructural changes in room temperature deposited functional ceramic thick films. [ABSTRACT FROM AUTHOR]

Aerosol deposition (AD) is a room‐temperature film deposition method for the fabrication of scalable ferroelectric ceramic films on different substrates, which is particularly appealing for thick film energy storage applications. However, the electrical and mechanical properties of AD ferroelectric films are not yet satisfactorily understood. Here, we report the dielectric, energy storage, and mechanical properties of aerosol‐deposited BaTiO3 (AD‐BT) thick films with nanosized grains by combining macroscopic electric measurements with indentation tests. We find that thermal annealing is an effective way to improve dielectric permittivity and polarization of the AD‐BT film, as well as to increase the hardness and Young's modulus of the film. However, crack formation in the annealed AD‐BT film is promoted in comparison to the as‐processed sample, suggesting that the interplay between the nanosized grains and release of the internal stress during annealing may have major consequences for the mechanical properties and hence should be taken into consideration in application. [ABSTRACT FROM AUTHOR]

External thermal, electrical, and mechanical fields can induce structural phase transitions in lead‐free Li‐modified Na0.5K0.5NbO3 ferroelectrics, which significantly influence the macroscopic electromechanical response. In particular, the relative stability of the polar monoclinic (or orthorhombic) and tetragonal phases under temperature and stress is critical to realize the ferroelectric and piezoelectric response. In this study, the effect of mechanical and thermal fields on the local structure in the vicinity of the monoclinic‐tetragonal (M‐T) phase boundary was investigated using a novel in situ combined uniaxial compressive stress‐ and temperature‐dependent Raman spectroscopy experimental arrangement. Experiments were performed up to 300°C and −200 MPa, clearly demonstrating stress‐induced M‐T phase transition in Li‐modified Na0.5K0.5NbO3. A stress‐temperature phase diagram has been established based on the change in vibrational modes. It was possible to correlate the relative permittivity singularities previously observed to a given stage of the M‐T phase transition using ratio between characteristic Raman band areas. In addition, the measurement method reported here can be applied to other functional ceramics to investigate the influence of mechanical fields on local structure. [ABSTRACT FROM AUTHOR]

External thermal, electrical, and mechanical fields can induce structural phase transitions in lead‐free Li‐modified Na0.5K0.5NbO3 ferroelectrics, which significantly influence the macroscopic electromechanical response. In particular, the relative stability of the polar monoclinic (or orthorhombic) and tetragonal phases under temperature and stress is critical to realize the ferroelectric and piezoelectric response. In this study, the effect of mechanical and thermal fields on the local structure in the vicinity of the monoclinic‐tetragonal (M‐T) phase boundary was investigated using a novel in situ combined uniaxial compressive stress‐ and temperature‐dependent Raman spectroscopy experimental arrangement. Experiments were performed up to 300°C and −200 MPa, clearly demonstrating stress‐induced M‐T phase transition in Li‐modified Na0.5K0.5NbO3. A stress‐temperature phase diagram has been established based on the change in vibrational modes. It was possible to correlate the relative permittivity singularities previously observed to a given stage of the M‐T phase transition using ratio between characteristic Raman band areas. In addition, the measurement method reported here can be applied to other functional ceramics to investigate the influence of mechanical fields on local structure. [ABSTRACT FROM AUTHOR]

Na1/2Bi1/2TiO3‐based relaxor ferroelectrics are extensively investigated for use in transduction applications because of their relatively large electromechanical properties. Integration of these materials into devices, however, requires better temperature stability in addition to electromechanical properties. This work demonstrates a novel approach to enhance the temperature stability of the long‐range ferroelectric order as well as to enhance electromechanical properties in a non‐ergodic relaxor 0.93(Na1/2Bi1/2)TiO3‐0.07BaTiO3 (NBT‐7BT) without changing the chemical composition through, for example, chemical substitutions or second phase particles. The approach involves the room temperature deposition of copper electrodes directly on the relaxor ceramic substrate using the aerosol deposition (AD) method. The collision of solid‐state particles with the substrate surface during AD results in large impact and residual stresses, inherent to the AD process, which are shown with piezo‐response force microscopy to induce long‐range ferroelectric domain ordering in non‐ergodic relaxor NBT‐7BT. Using Raman spectroscopy, the magnitude and depth profile of the stress‐induced transformation are determined. It is demonstrated that deposition‐induced stresses significantly increase the temperature stability of the electromechanical properties, where long‐range ferroelectric ordering is observed up to 150 °C, which is approximately 41 °C higher than NBT‐7BT samples without the AD processed electrode. Moreover, the AD treatment also facilitates ferroelectric domain switching at a lower electric field, enabling maximum polarization at a relatively lower field and an enhancement in the piezoelectric response. It is shown that the deposition‐induced stress is responsible for such an enhancement. Importantly, this impact‐stress‐driven tailoring of electromechanical properties can potentially be utilized for other functional ceramic materials as well, where internal residual stress can result in enhanced functional properties. [ABSTRACT FROM AUTHOR]

Aerosol deposition (AD) is a promising additive manufacturing method to fabricate low‐cost, scalable films at room temperature, but has not been considered for semiconductor processing, so far. The successful preparation of cesium lead tribromide (CsPbBr3) perovskite films on interdigitated indium tin oxide (ITO) electrodes by means of AD is reported here. The 20–35 µm thick layers are dense and have good adhesion to the substrate. The orthorhombic Pnma crystal structure of the precursor powder was retained during the deposition process with no signs of defect formation. The formation of electronic defects by photoluminescence spectroscopy is investigated and found slightly increased carrier recombination from defect sites for AD films compared to the powder. A nonuniform defect distribution across the layer, presumably induced by the impact of the semiconducting grains on the hard substrate surface, is revealed. The opto‐electronic properties of AD processed semiconducting films is further tested by electrical measurements and confirmed good semiconducting properties and high responsivity for the films. These results demonstrate that AD processing of metal halide perovskites is possible for opto‐electronic device manufacturing on 3D surfaces. It is believed that this work paves the way for the fabrication of previously unimaginable opto‐electronic devices by additive manufacturing. [ABSTRACT FROM AUTHOR]

Aerosol deposition (AD) is a dynamic loading process that can be envisioned as a shock wave loading, necessitating the consideration of the elastic/plastic response of solid materials. Due to the dynamic nature of this process, however, experimental determination of the local pressures during the deposition process is difficult. This work addresses this by investigating the compression and subsequent structure modification of a silicate glass after room‐temperature AD on a silicate glass substrate with Raman spectroscopy. Clear structural changes in the short‐ and middle‐range order of the silicate glass were observed, both as intertetrahedral angle distribution and as ring statistic. Therefore, the AD induced permanent densification of the glass, equivalent, in a hydrostatic approximation, to a minimal pressure of 10.5 ± 1.5 GPa during the film deposition process. Furthermore, the analysis of the Nd3+ photoluminescence of the 4F3/2 − 4I9/2 transition provided complementary information on the glass network modifications occurring during film formation. More than a pure hydrostatic densification, the AD seems to present a very intense shear deformation. This work opens up the perspective of evaluating the mechanical response of film‐substrate and of the particles themselves, and provides critical information on the mechanisms responsible for the AD film formation. [ABSTRACT FROM AUTHOR]

A novel technique for the rapid room‐temperature deposition of porous ceramic, glass, or metal thick films using the aerosol deposition (AD) method is presented. The process is based on the co‐deposition of the desired film material and a second water‐soluble constituent, resulting in a ceramic‐ceramic composite. Following the subsequent removal of water‐soluble end member, a network of pores is retained. To demonstrate the process, porous BaTiO3 thick films were fabricated through co‐deposition with NaCl. Microstructural images show the clear development of a porous structure, which was found to enhance the dielectric properties over dense thick films, possibly related to the lower extent of internal residual stress. This simple but highly effective porous structure fabrication can be applied to any film and substrate material stable in water and is promising for the application of AD‐processed films in gas sensors, solid oxide fuel cells, and humidity sensors. [ABSTRACT FROM AUTHOR]

Aerosol deposition is a feasible method of fabricating dense ceramic films at room temperature by the impact consolidation of submicron‐sized particles on ceramic, metal, glass, and polymer substrates at a rapid rate. Despite the potential usefulness of the aerosol deposition process, there are issues, such as deposition mechanisms and structure of the film‐substrate interface, that are not well understood. We have used complementary structural and microstructural analysis to capture the state of the substrate surface after the aerosol deposition process. The results reveal that modification of the substrate surface by the ejected submicron‐sized particles is essential for the formation of anchoring layer, thereby, a change in internal residual stress state and surface free energy of the substrate is required to deposit film using AD process. Our analysis also suggests that the adhesion between the metal substrate and ceramic particles is possibly contributed by both physical bonding and mechanical interlocking. [ABSTRACT FROM AUTHOR]

This work demonstrates the successful deposition of bioactive glass (BG) 45S5 coatings on various metallic and ceramic substrates at room temperature under low vacuum condition by using aerosol deposition (AD). This room temperature and particle impact consolidation-based deposition method enabled us to deposit well-adhered and dense BG coatings directly on metallic and ceramic substrates. In vitro tests with human osteoblast-like cells on substrates with a 45S5 BG coating demonstrated high cell activity on the surfaces. All tested materials exhibited high in vitro biocompatibility as no inhibition in cell proliferation could be observed. The utilization of AD process for achieving non-crystalline BG coatings is promising for practical bio-medical applications, e.g. , bioactive coatings on bioinert metallic and ceramic substrates. [ABSTRACT FROM AUTHOR]

Evolution of spectroscopic properties of a soda–lime silicate glass with different thermal history and under applied uniaxial stress was investigated using Raman and Brillouin spectroscopies as well as Nd3+ photoluminescence techniques. Samples of soda–lime silicate with a cooling rate from 6 × 10−4 to 650 K/min were prepared either by controlled cooling from the melt using a differential scanning calorimeter or by a conventional annealing procedure. Uniaxial stress effects in a range from 0 to −1.3 GPa were investigated in situ by compression of the glass cylinders. The spectroscopic observations of rearrangements in the network structure were related to the set cooling rates or the applied uniaxial stress to calculate an interrelated set of calibrations. Comparing the results from Raman and Brillouin spectroscopy with Nd3+ photoluminescence analysis, we find a linear dependence that can be used to identify uniaxial stress and cooling rate in any given combination concurrently. The interrelated calibrations and linear dependence models are established and evaluated, and equations relating the change of glass network due to effects of cooling rate or uniaxial stress are given. [ABSTRACT FROM AUTHOR]

The influence of stress on the phase boundaries of polycrystalline lead-free perovskite (1 − x)Ba(Zr0.2Ti0.8)O3–x(Ba0.7Ca0.3)TiO3 (x = 0.4, 0.5, and 0.6) was characterized through the temperature- and stress-dependent small-signal dielectric and piezoelectric response from − 150 to 200 °C under uniaxial compressive stress up to − 75 MPa. For all three compositions, the phase transition temperatures separating the rhombohedral, orthorhombic, tetragonal, and cubic phases were shifted to higher temperatures with an increase in the uniaxial mechanical loading, corresponding to a significant decrease in the dielectric and piezoelectric responses. Additional stress-dependent relative permittivity measurements up to − 260 MPa were conducted at four different constant temperatures (− 10, 10, 25, and 40 °C), revealing significant increases in the dielectric response, making these materials interesting for tunable dielectric applications. Furthermore, the stress-induced shift in phase transition temperatures was confirmed by in situ combined temperature- and stress-dependent Raman spectroscopy measurements under different constant uniaxial loads within the temperature range from 30 to 130 °C. [ABSTRACT FROM AUTHOR]