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Origin of Ferroelectricity in Epitaxial Si-doped HfO2 Films
摘要： HfO2-based unconventional ferroelectric (FE) materials were recently discovered and have attracted a great deal of attention in both academia and industry. The growth of epitaxial Si-doped HfO2 films has opened up a route to understand the mechanism of ferroelectricity. Here, we used pulsed laser deposition (PLD) to grow epitaxial Si-doped HfO2 films in different orientations of N-type SrTiO3 substrates. Using piezoforce microscopy, polar nanodomains can be written and read, and these domains are reversibly switched with a phase change of 180o. Films with different thicknesses displayed a coercive field Ec and a remnant polarization Pr of approximately 4～5 MV/cm and 8～32 μC/cm2, respectively. X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HRTEM) results identified that the as-grown Si-doped HfO2 films have strained fluorite structures. The ABAB stacking mode of the Hf atomic grid observed by HRTEM clearly demonstrates that the ferroelectricity originates from the noncentrosymmetric Pca21 polar structure. Combined with soft X-ray absorption spectra (XAS), it was found that the Pca21 ferroelectric crystal structure manifested as O sublattice distortion by the effect of interface strain and Si dopant interactions, resulting in further crystal-field splitting as a nanoscaled ferroelectric ordered state.
关键词： HRTEM,PLD,XRD,Ferroelectricity,PFM,XAS,Epitaxial Si-doped HfO2 thin films,N-type SrTiO3 substrates
更新于2025-11-14 17:04:02
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Operando XAS and NAP-XPS investigation of CO oxidation on meso- and nanoscale CoO catalysts
摘要： In contrast to Co3O4, CoO has been much less studied for CO oxidation. Herein, the phase changes of commercial mesoscopic CoO (particle size ?1 μm) and nanosized CoO (20–50 nm particle size), the latter prepared by vacuum reduction of commercial Co3O4, were examined by operando X-ray absorption (XAS) and near-ambient pressure X-ray photoemission (NAP-XPS) spectroscopy during CO oxidation, as well as ex situ by transmission electron microscopy and di?raction (TEM/SAED). Commercial mesoscopic CoO exhibited CO oxidation activity at ?200 °C, but even up to 530 °C in pure O2 no substantial (bulk) oxidation was observed by operando XAS, likely due to the large grains and bulk nature of CoO. After pre-oxidation at 400 C, electron di?raction detected thin surface layers of Co3O4. This increased activity but the activity of nanosized Co3O4 of equal surface area was still not reached. For nanosized CoO (surface layers on vacuum-reduced Co3O4), operando NAP-XPS/XAS, acquired during CO oxidation, revealed oxidation of CoO to Co3O4 above 150 °C, yielding the activity of nanosized Co3O4. Evidently, the nanoscale CoO shell on a Co3O4 core with small grains more easily and more completely transformed to Co3O4 than mesoscopic (bulk) CoO with large grains. Our study demonstrates how ?exible and dynamic surfaces of cobalt oxide materials adjust to various reaction environments, which also depends on grain size and morphology (bulk vs. thin layers), illustrating the importance of operando techniques to determine active catalyst phases under reaction conditions.
关键词： CO oxidation,CoO,Co3O4,NAP-XPS,XAS,TEM,Operando
更新于2025-09-23 15:23:52
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Development of a high temperature diamond anvil cell for x ray absorption experiments under extreme conditions
摘要： X-ray absorption spectroscopy (XAS) is presently a powerful and established tool to investigate solid and liquid matter at high pressure and high temperature (HP-HT). HP-HT XAS experiments rely on high pressure technology whose continuous development has extended the achievable range up to 100 GPa and more. In high pressure devices, high temperature conditions are typically obtained by using internal and external resistive heaters or by laser heating. We have recently developed a novel design for an internally heated diamond anvil cell (DAC) allowing XAS measurements under controlled high temperature conditions (tested up to about 1300 K). The sample in the new device can be rapidly heated or cooled (seconds or less) so the cell is suitable for studying melting/crystallization dynamics when coupled with a time-resolved XAS setup (second and sub-second ranges). Here we describe the internally heated DAC device which has been realized and tested in experiments on pure selenium at the energy dispersive ODE beamline of Synchrotron SOLEIL. We also present results obtained in XAS experiments of elemental Se using a large volume Paris-Edinburgh press, as an example of the relevance of structural studies of matter under extreme conditions.
关键词： high pressure,high temperature,DAC,Selenium,XAS
更新于2025-09-23 15:23:52
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Surface-interface analysis of In <sub/>x</sub> Ga <sub/>1-x</sub> As/InP heterostructure in positive and negative mismatch system
摘要： The change of In content in the InxGa1-xAs/InP system leads to the variation of the lattice constant and thereby to the negative mismatch between the base InP and the positive mismatch. Here, we studied the surface morphology and dislocation relationship of InxGa1-xAs/InP (100) in the positive and negative mismatch system by different characterization techniques. Under the same mismatch, the surface morphology and mass effect of negative mismatch were greater than those of positive mismatch. The reason was that in the negative mismatch system, during the film growth, the disorder degree at the interface increases, leading to an increase in dislocation density, meanwhile, the dislocation in the substrate more easily moved into the film, thus increasing the film and the dislocation density in it. Moreover, the mechanism of the buffer layer was also clarified. The addition of the buffer layer first limited the dislocation movement in the substrate, and secondly reduced the mismatch between the epitaxial layer and the substrate, thereby reducing mismatch dislocation.
关键词： surface/interface,lattice mismatch,InxGa1-xAs/InP,residual stress,dislocation
更新于2025-09-23 15:23:52
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Cu and Zr surface sites in photocatalytic activity of TiO2 nanoparticles: The effect of Zr distribution
摘要： The present work is focused on the role of ZrO2 modification in the performance of CuO modified TiO2. Zirconia loading leads to formation of more resistant photocatalytic layers compared to samples modified with only copper containing species. Surface modification of mixed phase TiO2 with CuO/ZrO2 improves the degradation of Reactive blue 19 dye under simulated solar irradiation. An in-depth investigation of the catalysts showed that in case of CuO/ZrO2 modification, the covering of the TiO2 surface with zirconium containing species prevents morphological and harmful energetic changes induced by copper species formed on the rutile TiO2 phase at a higher copper loading.
关键词： Hammett indicators,titanium dioxide,surface modification,XAS analysis,surface acidity
更新于2025-09-23 15:23:52
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Operando observation of chemical transformations of iridium oxide during photoelectrochemical water oxidation
摘要： Iridium oxide is one of the few catalysts capable of catalyzing the oxygen evolution reaction (OER) in both acidic and basic conditions. Understanding the mechanism of IrOx under realistic photoelectrochemical conditions is important for the development of integrated water splitting systems. Herein, we have developed a highly efficient OER photoanode in pH 1 aqueous solutions based on a sputtered IrOx film and a p+n-Si light absorber, interfaced with sputtered Au layer. Operando high energy resolution fluorescence detection X-ray absorption spectroscopy (HERFD XAS) was employed to monitor the oxidation state changes of IrOx during both electrochemical and photoelectrochemical (PEC) water oxidation reactions in pH 1 aqueous solutions. We observed a gradual increase of the average oxidation state of Ir with increasing anodic potential in the pre-catalytic region, followed by a reduction of Ir under O2 evolution conditions. Consistent results were obtained on dark anodes and illuminated photoanodes. However, when the thickness of IrO2 was increased to 2 and 3 nm, the spectral changes became much less pronounced and the reduction of Ir oxidation state after the OER onset was not observed. This is due to the lower surface to bulk ratio, where lattice oxygen sites in the bulk are not accessible for the formation of hydroxide. More generally, the operando method developed here can be extended to other materials, thereby providing a powerful tool for mechanism discovery and an enabling capability for catalyst design.
关键词： oxygen evolution reaction (OER),electrochemical and photoelectrochemical (PEC),high energy resolution fluorescence detection X-ray absorption spectroscopy (HERFD XAS),iridium oxide,Operando method
更新于2025-09-23 15:23:52
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Interface intermixing and interdiffusion characteristics in MOVPE grown spontaneous AlxGa1-xAs/GaAs (100) superlattice structures using high resolution X-ray diffraction
摘要： Thermal diffusion characteristics in naturally grown ultra-nanoscale superlattice structures have been studied. In absence of any suitable direct experimental tool due to the physical resolution limit, here we rely on the theoretical analysis of x-ray rocking curve simulations coupled with the diffusion equation to arrive at the diffusion characteristics across the interfaces of spontaneously grown AlGaAs/AlGaAs superlattice structures. The simulation approach presented here is a combination of a virtual interdiffusion code and a code on x-ray diffraction. We have obtained the variation in the actual diffusion coefficient as a function of time at different temperatures from the decay rates of the integrated satellite peak intensities. We have also found the diffusion coefficient to be highly nonlinear across the interface with time. The satellite decay equation could fit the experimental data taking the maximum Al composition alone at each time step. The pre exponential factor and the activation enthalpy values for interdiffusion are found out to be 0.17-0.25 cm2 /s and 0.5-0.6 eV for Al diffusion whereas 0.01-0.11 cm2/s and 3.45-3.5 eV for Ga diffusion, respectively in the studied temperature range of 500 oC to 700 oC. The interdiffusivity increases with temperature from 500 oC to 625 oC and decreases for further rise in temperature as the compositional contrast between the two layers decreases significantly at higher temperatures.
关键词： MOVPE,Interdiffusion,HTXRD,AlxGa1-xAs,Spontaneous superlattice
更新于2025-09-23 15:22:29
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Optical Properties of Energy-Dependent Effective Mass GaAs/GaxIn1?xAs and GaAs/AlxGa1?xAs Quantum Well Systems: A Shooting Method Study
摘要： In this paper, we study the effect of energy-dependent effective mass on optical properties of GaAs/GaxIn1?xAs and GaAs/AlxGa1?xAs quantum well systems through the compact density matrix approach. We solved the resulting non-linear Schro¨dinger equation by a simple shooting method and present the algorithm. We show that the energy-dependent effective mass effect is more important for systems with narrower quantum well systems. By an energy-dependent effective mass assumption, absorption coef?cient peak height increases with increasing the total system length L while in the constant effective mass limit, absorption coef?cient peak heights have not been in?uenced by changing L. In the GaAs/AlxGa1?xAs system, by increasing the number of wells, the linear absorption coef?cient amplitude at ?rst increases and then decreases in the ?xed effective mass approximation and monotonically decreases in the energy-dependent effective mass case. By increasing the number of wells, the linear absorption coef?cient peak position at ?rst shows a blue shift and then shows a redshift. In the GaAs/GaxIn1?xAs system, the situation is more complicated and it is described in more detail in the text. However, GaAs/GaxIn1?xAs quantum well systems have larger values of absorption coef?cient peak heights than GaAs/AlxGa1?xAs ones.
关键词： shooting method,GaAs/GaxIn1?xAs and GaAs/AlxGa1?xAs Quantum wells,refractive index changes,energy-dependent effective mass,absorption coef?cient
更新于2025-09-23 15:21:21
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In Situ SiO <sub/>2</sub> Passivation of Epitaxial (100) and (110)InGaAs by Exploiting TaSiO <sub/><i>x</i> </sub> Atomic Layer Deposition Process
摘要： In this work, an in situ SiO2 passivation technique using atomic layer deposition (ALD) during the growth of gate dielectric TaSiOx on solid-source molecular beam epitaxy grown (100)InxGa1?xAs and (110)InxGa1?xAs on InP substrates is reported. X-ray reciprocal space mapping demonstrated quasi-lattice matched InxGa1?xAs epitaxy on crystallographically oriented InP substrates. Cross-sectional transmission electron microscopy revealed sharp heterointerfaces between ALD TaSiOx and (100) and (110)InxGa1?xAs epilayers, wherein the presence of a consistent growth of an ～0.8 nm intentionally formed SiO2 interfacial passivating layer (IPL) is also observed on each of (100) and (110)InxGa1?xAs. X-ray photoelectron spectroscopy (XPS) revealed the incorporation of SiO2 in the composite TaSiOx, and valence band offset (ΔEV) values for TaSiOx relative to (100) and (110)InxGa1?xAs orientations of 2.52 ± 0.05 and 2.65 ± 0.05 eV, respectively, were extracted. The conduction band offset (ΔEC) was calculated to be 1.3 ± 0.1 eV for (100)InxGa1?xAs and 1.43 ± 0.1 eV for (110)InxGa1?xAs, using TaSiOx band gap values of 4.60 and 4.82 eV, respectively, determined from the fitted O 1s XPS loss spectra, and the literature-reported composition-dependent InxGa1?xAs band gap. The in situ passivation of InxGa1?xAs using SiO2 IPL during ALD of TaSiOx and the relatively large ΔEV and ΔEC values reported in this work are expected to aid in the future development of thermodynamically stable high-κ gate dielectrics on InxGa1?xAs with reduced gate leakage, particularly under low-power device operation.
关键词： in situ SiO2 passivation,atomic layer deposition,InxGa1?xAs,band alignment,TaSiOx,gate dielectric
更新于2025-09-23 15:21:01
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InAs on GaAs Photodetectors Using Thin InAlAs Graded Buffers and Their Application to Exceeding Short-Wave Infrared Imaging at 300?K
摘要： Short-wave infrared (SWIR) detectors and emitters have a high potential value in several fields of applications, including the internet of things (IoT) and advanced driver assistance systems (ADAS), gas sensing. Indium Gallium Arsenide (InGaAs) photodetectors are widely used in the SWIR region of 1–3 μm; however, they only capture a part of the region due to a cut-off wavelength of 1.7 μm. This study presents an InAs p-i-n photodetector grown on a GaAs substrate (001) by inserting 730-nm thick inxAl1?xAs graded and AlAs buffer layers between the InAs layer and the GaAs substrate. At room temperature, the fabricated InAs photodetector operated in an infrared range of approximately 1.5–4 μm and its detectivity (D*) was 1.65 × 108 cm · Hz1/2 · W?1 at 3.3 μm. To demonstrate performance, the Sherlock Holmes mapping images were obtained using the photodetector at room temperature.
关键词： InxAl1?xAs graded buffer,InAs p-i-n photodetector,GaAs substrate,room temperature operation,Short-wave infrared (SWIR),InGaAs photodetectors
更新于2025-09-11 14:15:04