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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Amorphous 2D Materials – A Novel Platform for Remote Epitaxy and Nanopatterned Epitaxy of III-V Semiconductors with Low Decomposition Temperatures

III-V semiconductor materials such as indium phosphide (InP) offer outstanding photonic properties that outperforms silicon, but the cost of these wafers is extremely expensive. Although reusing original wafers can effectively minimize the cost, current techniques for wafer recycling of these substrates add significant costs in fabrication, nullifying the cost savings by reusing the wafers. Besides, unlike other III-V materials such as gallium arsenide (GaAs), commonly used epitaxial lift-off method for wafer recycling is not well studied for materials like InP due to lack of lattice-matched sacrificial layers, which makes reusing these wafers more difficult. Remote epitaxy and nanopatterned epitaxy are newly discovered methods that enable single-crystal growth of III-V semiconductor thin films and easy exfoliation of these grown films, thus promising for a new cost-effective pathway of reusing wafers. However, previous methods of transferring two-dimensional (2D) materials, which use polymethyl methacrylate (PMMA) or metal stressor layers to transfer 2D materials grown on foreign substrates like copper (Cu) or silicon carbide (SiC), introduce defects and damages on the 2D layer and/or substrates during the transfer process. Remote epitaxial and nanopatterned epitaxial films grown on the damaged 2D layer/substrate suffer from lower crystal quality and imperfect exfoliation, which undermines wafer reusability and device performance. Here we report the MBE growth of amorphous boron nitride (a-BN) on InP wafers at low temperature that enabled improved quality of remote epitaxial and nanopatterned epitaxial films and their perfect exfoliation. We show fully covered a-BN on InP substrates despite their low decomposition temperatures. The surface of a-BN coated InP substrate remains smooth with a RMS roughness of around 3Å. We also demonstrate 100% coverage of single-crystal InP thin films grown on a-BN, with the film's quality significantly improved compared to the case of transferred 2D materials. In addition, the growth and exfoliation were successfully repeated multiple times, proving the feasibility for InP wafer recycling. Through this low temperature MBE growth approach with remote epitaxy and nanopatterned epitaxy, we successfully demonstrate large-scale flexible thin film exfoliation and recycling of InP substrates, which will lead to new opportunities in InP thin film-based photonics and novel heterostructures with significantly reduced cost.

Lu, Kuangye↗
DOE OSTI2022

Irradiation-induced amorphization of UO 2 films prepared by spraying-assisted combustion synthesis

Spraying-assisted combustion synthesis with uranyl nitrate – acetylacetone – 2-methoxyethanol solutions was used to prepare UO 2 films on an aluminum alloy substrate. The tuning of the spraying parameters and annealing temperatures allowed the preparation of UO 2 films with thicknesses varying from 10–300 nm and 5–10 nm UO 2 grain size. High-resolution electron microscopy and X-ray photoelectron spectroscopy showed that increasing the annealing temperature promotes Mg diffusion from the substrate into the films. The incorporation of Mg reduced the overall crystallinity of the films. The irradiation with Ar 2+ ions (1.7 MeV energy and a fluence of 2 × 10 16 ions/cm 2 ) did not degrade the quality of the films. However, the Mg content significantly influenced the irradiation-induced restructuring of the UO 2 films. Irradiated films with low or no Mg content exhibit high crystallinity, and the UO 2 /Al interfacial layer becomes highly porous. Films with higher Mg content are mostly amorphized after irradiation. The origin of irradiation-induced amorphization was related to the formation of Mg y U 1-y O 2±x solid solutions. Chemically complex, pore-free, and amorphous Mg-Al-O film/substrate interfacial layers enable continuous Mg diffusion during irradiation. As a result, the gradual increase in Mg amounts triggers irradiation-induced precipitation of a crystalline MgO-rich phase within the amorphous films.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

Proton diffusion and hydrogen/deuterium exchange in amorphous solid water at temperatures from 114 to 134 K

The reaction coefficient for hydrogen/deuterium (H/D) exchange and the diffusion of hydrated excess protons within amorphous solid water (ASW) are characterized as a function of temperature. For these experiments, water films are deposited on a Pt(111) substrate at 108 K, and reactions with pre-adsorbed hydrogen atoms produce hydrated protons. Upon heating, protons diffuse within the water, and H/D exchange occurs when they encounter D2O probe molecules deposited in the films. The time-dependent concentration of D2O is monitored with infrared spectroscopy, and it indicates the protons diffusion from the substrate and establish an equilibrium distribution prior to significant H/D exchange for temperatures 114 K ≤T≤ 134 K. By controlling the distance between the D2O molecules and the substrate, we probe the distribution of protons within the film. It decays as x−2 for the examined range of x (12–52 nm) due to the electric field that develops between the diffusing protons and their image charges in the metal substrate. This agrees with the theoretical distance scaling for the equilibrated proton concentration in a dielectric near a metal boundary. From the proton concentration and the measured D2O decay rate, a lower bound for the proton diffusion coefficient ranging from 10−20 m2/s at 114 K to 10−18 m2/s at 134 K is estimated. The diffusion coefficient has an activation energy of 0.40 eV, which is comparable to energies reported for molecular translations and rotations of H2O, suggesting they may play a critical role in the proton diffusion mechanism within ASW.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Morphology of Vapor-Deposited Acetonitrile Films

Crystalline acetonitrile has two polymorphs, a high temperature (HT) phase that is stable between 217 K and its melting point at 229 K, and a low temperature (LT) phase that is stable below 217 K. Solid acetonitrile films can be prepared by vapor deposition in an ultra-high vacuum chamber. To prevent sublimation of the film temperatures are often kept below 150 K. While the LT phase is thermodynamically favored at these low temperatures, such preparation usually results in the formation of the metastable HT polymorph. In this work we use reflection adsorption infrared spectroscopy (RAIRS) and temperature programmed desorption (TPD) experiments to investigate the effects of the deposition temperature and underlying substrate on the morphology of acetonitrile films prepared with molecular beam deposition. We obtained the elusive LT phase when dosing at 120 K on a graphene substrate and on a crystalline decane layer. Dosing acetonitrile on other surfaces produced the HT phase, as did annealing of amorphous films. We used TPD experiments to determine the Gibbs energy difference between the HT and LT phases. Our ΔG values agree with extrapolation of equilibrium calorimetry data. Furthermore, we also observed that acetonitrile films were amorphous when dosed at temperatures ≤ 60 K, and porous for temperatures ≤ 50 K.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Wafer-Scale Synthesis of 2D Materials by an Amorphous Phase-Mediated Crystallization Approach

The interest in the wafer-scale growth of two-dimensional (2D) materials, including transition metal dichalcogenides (TMDCs), has been rising for transitioning from lab-scale devices to commercial-scale systems. Among various synthesis techniques, physical vapor deposition, such as pulsed laser deposition (PLD), has shown promise for the wafer-scale growth of 2D materials. However, due to the high volatility of chalcogen atoms (e.g., S and Se), films deposited by PLD usually suffer from a lack of stoichiometry and chalcogen deficiency. To mitigate this issue, excess chalcogen is necessary during the deposition, which results in problems like uniformity or not being repeatable. This study demonstrates a condensed-phase or amorphous phase-mediated crystallization (APMC) approach for the wafer-scale synthesis of 2D materials. This method uses a room-temperature PLD process for the deposition and formation of amorphous precursors with controlled thicknesses, followed by a post-deposition crystallization process to convert the amorphous materials to crystalline structures. This approach maintains the stoichiometry of the deposited materials throughout the deposition and crystallization process and enables the large-scale synthesis of crystalline 2D materials (e.g., MoS 2 and WSe 2 ) on Si/SiO 2 substrates, which is critical for future wafer-scale electronics. We show that the thickness of the layers can be digitally controlled by the number of laser pulses during the PLD phase. Optical spectroscopy is used to monitor the crystallization dynamics of amorphous layers as a function of annealing temperature. The crystalline quality, domain sizes, and the number of layers were explored using nanoscale and atomistic characterization (e.g., AFM, STEM, and EDS) along with electrical characterization to explore process–structure–performance relationships. Finally, this growth technique is a promising method that could potentially be adopted in conventional semiconductor industries for wafer-scale manufacturing of next-generation electronic and optoelectronic devices.

2D electronics↗
DOE OSTI2023

Estimating viscosity of individual substrate-deposited particles from measurements of their height-to-width ratios

Airborne particles alter the radiative forcing of climate and have further consequences on air visibility, atmospheric chemistry, and human health. Recent studies reported the existence of highly viscous semisolid and even solid amorphous organic aerosol (OA) particles. Particle viscosity has an impact on the heterogeneous chemistry, gas-particle partitioning, and ice nucleation properties. Consequently, variations in particle viscosity must be considered when predicting the atmospheric impact of OA. Here, in this work, we use scanning electron microscopy (SEM) and scanning transmission X-ray microscopy (STXM) to estimate the viscosity of individual particles deposited on substrates based on their characteristic height-to-width ratios, which are affected by changes in morphology upon deposition. The height-to-width ratios obtained from SEM and STXM exhibit a strong correlation, demonstrating that both imaging approaches can be applied separately for viscosity assessment of the substrate-deposited particles. While these metrics are largely qualitative, this method enables rapid assessment of particle viscosity ranges, distinguishing between semisolid (>10 10 Pa·s), viscous (10 4– 10 8 Pa·s), and liquid (10°–10 1 Pa·s) particles within ensembles of ambient particles collected for microscopy studies.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Improving stability of ALD ZrN thin film coatings over U-Mo dispersion fuel

Atomic layer deposition (ALD) of ZrN is a candidate technology for coating U-Mo dispersion fuel as a diffusion barrier coating. During the early development stages of the coating the ZrN deposition showed to be mechanically unstable and ultimately resulted in spalling. Based on experimental outcomes it was found that instabillity can be eliminated through the introduction of a thin amorphous (a) Al 2 O 3 interlayer coating deposited in between the ~1-μm thick ZrN and the U-Mo. substrate. To elucidate these findings simulations were performed with density functional theory (DFT) to measure work of adhesions at different interfaces while finite element modeling (FEM) was performed to measure the residual stress distribution. DFT indicated that the ZrN coating deposited over (a)-Al 2 O 3 is ~2.5 times stronger when compared to direct deposition over U or UO 2 substrate. While calculations from FEM recognized; (1) large stress concentrations can originate from the irregularly distributed native surface oxides (UO 2 ) over U-Mo and (2) stress concentrations can be reduced if those surface UO 2 can be modified to a uniform layer (achieved after application of a 8 nm (a)-Al 2 O 3 interlayer). These results provided explanations and confirmed the role played by interlayer in eliminating the original mechanical instability of the ZrN.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Morphology, microstructure, and doping behaviour: A comparison between different deposition methods for poly-Si/SiO x passivating contacts

In this work, we study how crystallographic structures, optoelectronic properties, and nanoscale surface morphologies of ex situ phosphorus-doped polycrystalline silicon (poly-Si)/SiO x passivating contacts, formed by different deposition methods (sputtering, plasma-enhanced chemical vapour deposition [PECVD], and low-pressure chemical vapour deposition [LPCVD]), are investigated and compared. Across all these deposition technologies, we noted the same trend: higher diffusion temperatures yield films that are more crystalline but that have rougher surface morphologies due to bigger surface crystal grains. Also, the recrystallization process of the as-deposited Si films starts from the SiO x interface, rather than from the film surface and bulk. However, there are some distinct differences among these technologies. First, the LPCVD method yields the lowest deposition rate, roughest surfaces, and smallest degree of crystallinity on finished poly-Si films. In contrast, the PECVD method has the highest deposition rate and smoothest surfaces for both as-deposited Si and annealed poly-Si films. Second, as-deposited sputtered and PECVD Si films contain only an amorphous phase, whereas as-deposited LPCVD films already has some crystalline phase. Third, the LPCVD phosphorus in-diffusion into the substrate depends strongly on the initial film thickness, whereas for the other two methods, it is weakly dependent on thickness. Finally, the passivation quality of every poly-Si film type has different responses to the film thickness and diffusion temperature, suggesting that the ex situ doping optimization should be performed independently.

14 SOLAR ENERGY↗
DOE OSTI2020

Ultrathin high- κ antimony oxide single crystals

Ultrathin oxides have been reported to possess excellent properties in electronic, magnetic, optical, and catalytic fields. However, the current and primary approaches toward the preparation of ultrathin oxides are only applicable to amorphous or polycrystalline oxide nanosheets or films. Here, we successfully synthesize high-quality ultrathin antimony oxide single crystals via a substrate-buffer-controlled chemical vapor deposition strategy. The as-obtained ultrathin antimony oxide single crystals exhibit high dielectric constant (~100) and large breakdown voltage (~5.7 GVm -1 ). Such a strategy can also be utilized to fabricate other ultrathin oxides, opening up an avenue in broadening the applicaitons of ultrathin oxides in many emerging fields.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Perspective on solid-phase epitaxy as a method for searching novel topological phases in pyrochlore iridate thin films

Pyrochlore iridates exhibit various novel topological phenomena due to their topology and electron correlation. Notably, pyrochlore iridate was the first proposed material system shown to host the time-reversal symmetry broken Weyl semimetal phase. After this profound theoretical proposal, extensive experimental attempts have been made to synthesize high-quality samples in both bulk and film forms. In particular, adjusting thin film geometry represents a practical way to tune the U/ t ( U: Coulomb interaction and t: for hopping parameter) and identify the various topological phases in the regime U ~ λ ( λ: spin–orbit interaction). However, the instability of pyrochlore iridates at high temperature and low oxygen pressure has long been a barrier to growing pyrochlore iridate thin films by conventional film growth methods. To overcome this, pyrochlore iridate films have often been grown by the solid-phase epitaxy method, which uses a metastable amorphous layer grown at low temperature. During a high temperature post-annealing process, the layer in contact with a single crystalline substrate will crystallize epitaxially in the solid state by rearranging atoms at the interface. Here, we present a perspective on the solid-phase epitaxy as a method to synthesize epitaxial pyrochlore iridate thin films and a way to search for novel correlated phenomena.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Comparative Studies of Optoelectronic Properties, Structures, and Surface Morphologies for Phosphorus-Doped Poly-Si/SiOx Passivating Contacts

We investigated and compared optoelectronic properties, crystallographic structures, and nanoscale surface morphologies of ex-situ phosphorus-doped polycrystalline silicon (poly-Si)/SiO x passivating contacts, formed by different deposition methods (sputtering, plasma-enhanced chemical vapour deposition (PECVD), and low-pressure chemical vapour deposition (LPCVD)). Across all these deposition technologies, a similar trend is observed: higher diffusion temperatures yield films that are more crystalline but have rougher surface morphologies due to bigger surface crystal grains. Also, the recrystallization process of the as-deposited Si films starts from the SiO x interface, rather than from the film surface and bulk. However, there are some distinct differences among these technologies. Firstly, the LPCVD method yields the roughest surface and smallest degree of crystallinity on finished poly-Si films. In contrast, the PECVD method has the smoothest surface for both as-deposited Si and annealed poly-Si films. Secondly, as-deposited sputtered and PECVD Si films contain only an amorphous phase whereas as-deposited LPCVD films has already had some crystalline phase. Thirdly, the LPCVD phosphorus in-diffusion into the substrate depends strongly on the initial film thickness, whereas for the other two methods it is weakly dependent on thickness.

crystallographic structures↗
DOE OSTI2022

Lytic polysaccharide monooxygenase increases cellobiohydrolases activity by promoting decrystallization of cellulose surface

Efficient depolymerization of crystalline cellulose requires cooperation between multiple cellulolytic enzymes. Through biochemical approaches, molecular dynamics (MD) simulation, and single-molecule observations using high-speed atomic force microscopy (HS-AFM), we quantify and track synergistic activity for cellobiohydrolases (CBHs) with a lytic polysaccharide monooxygenase (LPMO) from Phanerochaete chrysosporium. Increasing concentrations of LPMO (AA9D) increased the activity of a glycoside hydrolase family 6 CBH, Cel6A, whereas the activity of a family 7 CBH (Cel7D) was enhanced only at lower concentrations of AA9D. MD simulation suggests that the result of AA9D action to produce chain breaks in crystalline cellulose can oxidatively disturb the crystalline surface by disrupting hydrogen bonds. HS-AFM observations showed that AA9D increased the number of Cel7D molecules moving on the substrate surface and increased the processivity of Cel7D, thereby increasing the depolymerization performance, suggesting that AA9D not only generates chain ends but also amorphizes the crystalline surface, thereby increasing the activity of CBHs.

09 BIOMASS FUELS↗
DOE OSTI2026

Synthesis and composition control of epitaxial FeWO4 thin films using pulsed laser deposition

We report the growth of epitaxial FeWO4 thin films on c-plane sapphire via pulsed laser deposition using a Fe 2 O 3 /WO 3 target ablated in an O 2 atmosphere. At a constant O 2 pressure of 1 mTorr, x-ray diffraction (XRD) confirms FeWO 4 as the major crystalline phase for substrate temperatures from 500 to 800 °C. As temperature increases, x-ray fluorescence (XRF) shows the Fe/W ratio remains nearly constant at 0.90 ± 0.02, while x-ray photoelectron spectroscopy (XPS) shows Fe 3+ to Fe 2+ conversion increases from 20% to 35%. Morphological analysis reveals phase separation, likely of amorphous Fe 3+ oxide from crystalline FeWO 4 , increasing with Fe 3+ conversion. This is attributed to an O-rich laser ablated flux, where conversion is driven by the Arrhenius temperature dependence of Fe 3+ → Fe 2+ reduction on the film surface. At a constant substrate temperature of 750 °C, XRD confirms FeWO 4 formation for O 2 pressures from 0.5 to 10 mTorr. As pressure increases, XRF shows the Fe/W ratio decreases from 0.98 to 0.70, while XPS shows Fe 3+ conversion rises from 15% to 70%. Morphology shows phase separation decreasing with increasing Fe 3+ conversion. This is attributed to scattering, where higher O 2 pressure makes the laser ablated flux O-deficient relative to Fe and W, facilitating Fe 2+ formation. Films with Fe 3+ conversion above ∼30% and Fe/W ratios from 0.86 to 0.96 exhibit FeWO 4 optical and electronic properties suitable for photoanode applications.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Unraveling the Highly Plastic Behavior of ALD-Aluminum Oxide Encapsulations by Small-Scale Tensile Testing

We present a study directly measuring the electron-beam-induced plasticity of amorphous Al 2 O 3 coatings. Core–shell nanostructures are employed as small-scale model systems for two-dimensional coatings made by atomic layer deposition (ALD). Copper nanowires (NWs) are used as substrates for ALD deposition, representing a model system for interconnects commonly found in integrated circuits. Experiments are performed in situ in a transmission electron microscope (TEM) and further analyzed with electron energy loss spectroscopy (EELS). Our in situ TEM tensile experiments reveal the highly plastic behavior of the ALD shell, which withstands a maximum strain of 188%. Comparable samples under beam-off conditions show a brittle fracture, which underlines the effect of electron irradiation. The electron-beam-activated bond switching within the amorphous network enables compensation of the applied tensile strain, leading to viscous flow. By incorporating an intermediate nanocrystalline layer within the Al 2 O 3 shell, the plasticity is suppressed and brittle fracture occurs. This work directly demonstrates the tuning of mechanical properties in amorphous ALD structures through electron irradiation.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Au and Pt Diffusion in Electrodeposited Amorphous Sb 2 Te 3 Thin Films

Amorphous Sb 2 Te 3 thin films are synthesized using electrodeposition in different thicknesses to explore their solid electrolytic nature with respect to some noble metals. Au and Pt are used as the substrate materials and thermally diffused into the Sb 2 Te 3 films under passivated and nonpassivated conditions. Rutherford backscattering spectrometry is used to study the Au and Pt diffusion into the films as a function of depth. It is found that Au diffuses into the Sb 2 Te 3 thin films even at room temperature. In contrast, there is no observable diffusion of Pt at room temperature. At a higher temperature (i.e., 200 °C), both Au and Pt diffuse into the Sb 2 Te 3 thin films and Au diffusion is more significant than Pt. Overall, the findings suggest that amorphous Sb 2 Te 3 can be used as a good solid electrolyte to permit the diffusion of some noble metals such as Au and Pt.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Local Thermochemical Mechanisms in Direct Solar Graphite Synthesis from Methane

Methane pyrolysis is known to produce hydrogen and solid carbon in a variety of thermal processes. However, the generated carbon product typically belongs to a low-value amorphous type. Here, we elucidate the thermochemical mechanisms of a reaction that produces high-quality graphite via direct solar methane pyrolysis on a porous substrate. By comparing graphite deposition rates and local reaction zone temperatures of exposed and shadowed regions from the same experiment, we clarify the effects of thermolysis and photolysis in this emission-free process that both decarbonizes a fuel and produces a critical material for the sustainable energy transition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Hardware, methodology and applications of 2 + D backscatter Mössbauer spectroscopy with simultaneous x-ray and γ-ray detection

Abstract A unique method is presented for the acquisition and analysis of 57 Fe backscatter Mössbauer spectra with simultaneous detection of the resonant 14.4 keV γ -rays and the characteristic 6.4 keV x-rays, using a custom-built multi-parameter analyser constructed on the basis of commercial analogue to digital converters and high-speed digital latches. The system allows for the simultaneous registration of Doppler-modulation velocities and photon energies, with up to 4096 and 8192 digital channels respectively. This arrangement is in contrast to most related systems, which detect at a single narrow energy window per detector. Samples of arbitrary atomic structure, morphology and surface topography can be studied without altering the setup or the analysis procedure, provided that the samples are at least micrometre sized. The hardware and software that are used to acquire data with minimal dead time are described and the custom and self-contained methods for post-measurement energy discrimination, background correction and velocity-axis folding are discussed. The data are fit using a general Hamiltonian model for the nuclear energy levels of 57 Fe and a quantum mechanical description of the angular momentum coupling is utilised, with consideration of the crystalline and chemical disorder of the sample under examination. Three examples of distinct magnetic systems, with thicknesses ranging from 5 μ m to 6 mm, that were studied using this method are presented, these are: an amorphous CoFeB-based ribbon with ultra-soft coercivity for high-frequency applications, magnetically hard Nd-Fe-B thick films on Si substrates, examined in both as-deposited and annealed states, and a sample from the nickel-rich iron meteorite NWA 6259 that contains the atomically ordered, elevated coercivity, L 1 0 phase of FeNi, tetrataenite. The wide applicability and usefulness of this method is thus demonstrated on three distinct sample morphologies that required little to no surface preparation prior to examination.

Engineering↗
DOE OSTI2022

Phase transformation and growth mechanism of RF sputtered ferroelectric lead scandium tantalate (PbSc 0.5 Ta 0.5 O 3 ) films

Lead scandium tantalate (PbSc 0.5 Ta 0.5 O 3 , PST), an order/disorder ferroelectric, is a potential candidate for electrocaloric cooling and pyroelectric infrared (IR) detector. In this work, we report the phase transformation kinetics from two series of samples containing pure amorphous and mixture of amorphous and pyrochlore to desired perovskite phase using postdeposition rapid thermal processing (RTP) as well as growth mechanism of RF sputtered PST thin films using excess lead target on platinized silicon (Pt/Ti/SiO 2 /Si) substrates. We find that small changes in the temperature ramp have a large effect on the degree of perovskite conversion (ferroelectric phase), orientation (crystallographic texture), and long-range order parameter (< S 111 >). Through isothermal annealing, we obtained optimal perovskite phase at ≥700°C temperature. The phase transformation is characterized by spontaneous formation of center-type in-plane radial rosette-like structures revealed by scanning electron microscopy. The PST perovskite crystallites were found to coexist with pyrochlore in RTP annealed films. The volume fractions for perovskite and pyrochlore phase were obtained from the analysis of “rosettes” and respective X-ray diffraction intensities which helped to determine various parameters associated with phase kinetics (n, k, and activation energy, Ea) and accompanying growth. The effective activation energies of perovskite transition and growth were found to be 332 ± 11 kJ/mol (345 ± 11 kJ/mol) and 114 ± 10 kJ/mol (122 ± 10 kJ/mol), respectively, for pure amorphous only (and mixed amorphous and pyrochlore) phase following nucleation-growth controlled Avrami's equation. A linear growth rate (n~1) for the perovskite phase indicates predominant interface-controlled process and diffusion-limited phenomena thus inhibiting rosette size owing to reactant depletion and soft impingement at the grain boundary. However, the growth behavior is isotropic in two-dimension parallel to the plane of the substrates for both sample series. Furthermore, lead loss was severe for in-situ growth and RTP combined with conventional furnace annealing than those of RTP only films, which were closer to stoichiometric albeit with excess lead and marginal oxygen vacancies (V o ).

36 MATERIALS SCIENCE↗