Lattice Inhomogeneity Research Articles

Tensile Microstrain Fluctuations in the BaPbO Units in Superconducting BaPb1−xBixO3 by Scanning Dispersive Micro-XANES

BaPb1−xBixO3 (BPBO) bismuthate, showing high TC superconductivity for 0.05 < x < 0.35, is an archetypal system for studying the complex inhomogeneity of perovskite lattice favoring the emergence of quantum coherence, called the superstripes phase. Local lattice fluctuations, detected by EXAFS; nanoscale stripes, detected by electron microscopy; and two competing crystalline structures, detected by diffraction, are known to characterize the superconducting phase. At nanoscale [BaBiO3] centered nanoscale units (BBO) coexist with BaPbO3 centered (BPO) units in the BPBO perovskite; therefore, we expect a tensile microstrain in BPO units due the misfit strain between the two different lattices. Here, we report the measurement of the spatial micro-fluctuations of the local tensile microstrain ε in the BaPO units in superconducting Ba(Pb1−xBix)O3 crystals with x1 = 0.19 an x2 = 0.28. We show here the feasibility of applying the scanning dispersive micro-X-ray absorption near edge structure (SdμXANES) technique, using focused synchrotron radiation, to probe the microscale spatial fluctuations of the microstrain in BPO units. This unconventional real-space SdμXANES microscopy at the Pb L3 edge has been collected in the dispersive mode. Our experimental method allows us to measure either the local Bi chemical concentration x and the local lattice microstrain of local BBO and BPO units. The 5 × 5 micron-size spots from the focused X-ray beam allowed us to obtain maps of 1600 points covering an area of 200 × 200 microns. The mapping shows a substantial difference between the spatial fluctuations of the microstrain ε and the chemical inhomogeneity x. Moreover, we show the different relations ε(x) in samples with lower (x1 = 0.19) and higher (x2 = 0.28) doping respect to the optimum doping (x = 0.25).

Combined impact of B2H6 flow and growth temperature on morphological, structural, optical, and electrical properties of MOCVD-grown B(In)GaAs heterostructures designed for optoelectronics

BGaAs/GaAs epilayers and BInGaAs/GaAs quantum well (QW) have been prepared using metal–organic chemical vapor deposition under different growth conditions, and their physical and structural properties have been examined. SEM-EDS investigation showed a dependence of surface properties of the ternary compound on the growth conditions. High-resolution X-ray diffraction evidenced a tensile strain for the ternary alloys whatever the growth condition, while the quaternary QW always shows a compressive strain state. Room temperature optical absorption allowed to follow the variation of the bandgap with boron incorporation. Photoluminescence measurements confirmed the carrier-localization phenomenon and its dependence with the growth conditions. Deposition temperature and diborane (B2H6) flow rate are with particularly significant effects on the optical properties: lower diborane flow rate and high growth temperature enhance the radiative emission. Computer simulation using localized state ensemble model quantitatively relates the lattice inhomogeneity to the optical properties and suggests a way to engineer the localization phenomenon and avoid clustering effects. Electrical investigations by current–voltage, capacitance and conductance methods have been performed for the first time on selected BGaAs samples. The ideality factor of Schottky barriers has been determined, while their height and film doping level could only be approximately estimated. Such physical properties make boron-based alloys very promising for applications in multijunction solar cells.

Chemical free energy profiles for martensitic transformation of CuAlNi at finite temperatures

The free energy profile for atomistic configurations of a given deformation process is the key to understand behaviors of materials at all scales. The martensitic transformation of CuAlNi at finite temperatures features a twinning deformation process. The chemical free energy profiles for intermediate twinning configurations at finite temperatures are constructed in two steps incorporating an internal variable describing the twinning microstructure development in the martensitic transformation process. The first takes place at 0 K where one unique lattice parameter is constrained to obtain the twinned configurations with different levels of twinning shear via first-principles density functional theory (DFT) optimizations. Resultant free energy profiles from a hybrid-atom model and three localized lattice models show that the lattice inhomogeneity has a strong connection with the twinning growth in the MT process. The second covers a range from 0 K to a finite temperature with lattice sizes fixed. The chemical free energy profiles of martensitic microstructures at finite temperatures obtained via the corresponding thermodynamic analysis differ the standard Landau double-well potential significantly on symmetry and curvature, which are responsible for the dynamics of twinning development. The method proposed can be applied to other martensitic material systems.

Flexoelectricity in thin films and membranes of complex oxides

Flexoelectricity describes the generation of electric polarization in response to inhomogeneous strain, i.e., strain gradient, in all dielectrics. Importantly, strain gradients are inversely scaled to the material dimension so that more prominent and exotic phenomena can be envisioned at the nanoscale, based on flexoelectricity. In particular, in complex oxides, such a large lattice inhomogeneity can also host a rich spectrum of properties and functionalities, via a subtle interplay with charge, spin, and orbital. Here, motivated by advances in nanoscale thin-film and membrane syntheses of complex oxides, we present the frontiers and challenges of flexoelectricity. Together with the advanced synthesis techniques, state-of-the-art experimental nano-techniques will continue to reveal hitherto hidden functionalities through flexoelectricity. Meanwhile, further breakthroughs in the research of flexoelectricity will require consistency between theory and experiment and will rely on the versatile exploitation of large strain gradients in nanoscale complex oxides.

Superconductivity in Quantum Complex Matter: the Superstripes Landscape

While in XX century the theory of superconductivity has focused on a homogeneous metal with a rigid lattice which can be reduced to a single effective conduction band in the dirty limit. Today in the XXI century, the physics of superconductivity is focusing on complexity of quantum matter where novel quantum functionalities with lattice inhomogeneity at nanoscale (between 1 nm and 100 nm) and at mesoscopic scale (in the range 100-10000 nm), where the electronic structure need to be described by multiple Fermi surfaces and multiple gaps in the superconducting phase in the clean limit. The present issue of Journal of superconductivity and Novel magnetism collects papers presented at the International Conference Superstripes 2019 which was held on June 23-29, 2019, in Ischia Island, Italy. The series of Stripes conference started on Dec 8 1996 and it has contributed to scientific advances in the new physics of superconductivity in quantum complex systems in these last 23 years where polarons, strain, multigap superconductivity, exchange interaction between condensates, granular superconductivity and percolation play a key role. The articles collected in this issue cover hot topics of the new quantum physics of complex matter including the mechanism of high temperature superconductivity, complex magnetic orders and orbital physics in strongly correlated materials which have been growing rapidly in these last two years opening new perspectives also in mesoscopic quantum engineering.

Ferromagnetic resonance in nanotwinned Ni–Mn–Ga film undergoing martensitic transformation

The ferromagnetic resonance (FMR) in the shape memory alloys (SMAs) exhibiting structural cubic-tetragonal phase transition has been studied. The influence of instability and spatial inhomogeneity of crystal lattice on the FMR spectra of twinned ferromagnetic SMAs films has been analyzed using statistical model of ferromagnetic martensite. It has been shown that the abnormally strong temperature dependence of lattice parameters of martensitic film gives a noticeable contribution to the temperature dependence of the resonance value of external magnetic field. The narrowing of the resonance peak, which had been experimentally observed on cooling of the film slightly below the Curie temperature, has been explained. It is argued that the martensitic films are good candidates for the experimental study of local elastic strains influence on the shape of the FMR peak.

On the interstitial induced lattice inhomogeneities in nitrogen-expanded austenite

Lattice inhomogeneities, i.e. nitrogen interstitial-induced hexagonal-close-packed martensite (HCP-εN) and shear bands, can form in face-centred cubic nitrogen-expanded austenite (FCC-γN) synthesised on Fe-Cr-Mn and Fe-Cr-Ni austenitic stainless steel (ASS) using triode-plasma nitriding (TPN). Homogenous elemental distribution between HCP-εN and FCC-γN supports the displacive shear transformation mechanism proposed for a high-Mn, low stacking fault energy ASS under nitrogen interstitial-induced deformation. While resulting from transformation-induced plasticity, HCP-εN exhibits similar lattice expansion behaviour to the parent FCC-γN. However, inhomogeneous elemental distributions in the shear bands formed in γN layers on a 400°C TPN-treated high-Ni ASS indicate local migration of substitutional elements.

Synthesis Techniques of Nickel Substituted Cobalt Ferrites – An Investigative Study Using Structural Data

Structural properties of nickel-substituted cobalt ferrite nano-particles Ni x Co 1-x Fe 2 O 4 (x=0.2,0.8) synthesized using two different methods, namely combustion and co-precipitation are studied. The structural parameters of Nickel-substituted Cobalt ferrite nano-particles confirm the formation of nano-sized particles of cubic spinel structure. Lattice parameters, density, particle size and inhomogeneity are determined while Attenuated total reflectance (ATR-IR) spectroscopy and scanning electron microscope images are studied. The ATR-IR spectra show transmission peaks, in the range around 600cm -1 and 400 cm -1 which respectively arise from tetrahedral and octahedral interstitial sites in the spinel lattice and found cationic exchanges between the lattices of these sites. The studies reveal that the sol–gel auto combustion method can be preferred to the co-precipitation method for producing single phase nano particles with smaller crystallite size

Evolution of a Novel Ribbon Phase in Optimally Doped Bi2Sr2CaCu2O8+δ at High Pressure and Its Implication to High- TC Superconductivity.

One challenge in studying high-temperature superconductivity (HTSC) stems from a lack of direct experimental evidence linking lattice inhomogeneity and superconductivity. Here, we apply synchrotron hard X-ray nanoimaging and small-angle scattering to reveal a novel micron-scaled ribbon phase in optimally doped Bi2Sr2CaCu2O8+δ (Bi-2212, with δ = 0.1). The morphology of the ribbon-like phase evolves simultaneously with the dome-shaped TC behavior under pressure. X-ray absorption studies show that the increasing of TC is associated with oxygen-hole redistribution in the CuO2 plan, while TC starts to decrease with pressure when oxygen holes become immobile. Additional X-ray irradiation experiments reveal that nanoscaled short-range ordering of oxygen vacancies could further lower TC, which indicates that the optimal TC is affected not only by an optimal morphology of the ribbon phase, but also an optimal distribution of oxygen vacancies. Our studies thereby provide for the first time compelling experimental evidence correlating the TCwith micron to nanoscale inhomogeneity.

Quantitative Characterization of the Nanoscale Local Lattice Strain Induced by Sr Dopants in La_{1.92}Sr_{0.08}CuO_{4}.

The nanometer scale lattice deformation brought about by the dopants in the high temperature superconducting cuprate La_{2-x}Sr_{x}CuO_{4} (x=0.08) was investigated by measuring the associated x-ray diffuse scattering around multiple Bragg peaks. A characteristic diffuse scattering pattern was observed, which can be well described by continuum elastic theory. With the fitted dipole force parameters, the acoustic-type lattice deformation pattern was reconstructed and found to be of similar size to lattice thermal vibration at 7K. Our results address the long-term concern of dopant introduced local lattice inhomogeneity, and show that the associated nanometer scale lattice deformation is marginal and cannot, alone, be responsible for the patched variation in the spectral gaps observed with scanning tunneling microscopy in the cuprates.

Mo-Al co-doped VO2(B) thin films: CVD synthesis, thermal sensitive properties, synchrotron radiation photoelectron and absorption spectroscopy study

Endowing vanadium dioxide (VO2) thin films with excellent thermal sensitive performance is greatly desired for application in uncooled infrared (IR) detectors. Here, we demonstrate a strategy of co-doping by using a simple and feasible CVD method to synthesize Mo-Al-doped VO2(B) thin films with high temperature-coefficient-of-resistance (TCR, −3.6%/K) and favorable square resistances (16.2 kΩ). Both the TCR and resistance are superior to that of undoped and Al-doped VO2(B) thin film, and the TCR is larger than that of Mo-doped VO2(B) thin film. The underlying microscopic mechanism for the performance improvement might be that Mo-Al co-doping creates less lattice deformation, strain and inhomogeneity of carrier concentration due to dimension and charge compensation than that of single-doping and the partly release of 3d electrons around V4+-V4+ pairs in co-doping films. Besides, the special two-dimensional octahedral structure of monoclinic (C2/m) VO2(B) favors the strain control with doping. The films have been subjected to synchrotron radiation based X-ray photoelectron spectroscopy (SRPES) and X-ray absorption near edge structure (XANES) techniques to study the local atomic and electronic structure around V ions. The results indicated that the dopants of Mo and Al were incorporated into the VO2 lattice and occupied some of the V lattice sites, resulting in the formation of the V1-x-yMoxAlyO2 substitution solid solution. V L-edge and O K-edge XAS results identically verified that Mo-Al co-doping might create the least lattice deformation in films. Hence, the high performance of films proves that the co-doping strategy is suitable for uncooled infrared detector applications.

Nature and evolution of incommensurate charge order in manganites visualized with cryogenic scanning transmission electron microscopy

Incommensurate charge order in hole-doped oxides is intertwined with exotic phenomena such as colossal magnetoresistance, high-temperature superconductivity, and electronic nematicity. Here, we map, at atomic resolution, the nature of incommensurate charge-lattice order in a manganite using scanning transmission electron microscopy at room temperature and cryogenic temperature ([Formula: see text]93 K). In diffraction, the ordering wave vector changes upon cooling, a behavior typically associated with incommensurate order. However, using real space measurements, we discover that the ordered state forms lattice-locked regions over a few wavelengths interspersed with phase defects and changing periodicity. The cations undergo picometer-scale ([Formula: see text]6 pm to 11 pm) transverse displacements, suggesting that charge-lattice coupling is strong. We further unearth phase inhomogeneity in the periodic lattice displacements at room temperature, and emergent phase coherence at 93 K. Such local phase variations govern the long-range correlations of the charge-ordered state and locally change the periodicity of the modulations, resulting in wave vector shifts in reciprocal space. These atomically resolved observations underscore the importance of lattice coupling and phase inhomogeneity, and provide a microscopic explanation for putative "incommensurate" order in hole-doped oxides.

Compositional effect on dielectric and ferroelectric properties of lead free Zr modified BNT ceramic

ABSTRACTThe effect of zirconium substitution on dielectric and ferroelectric properties of Bi0.5Na0.5Ti1-xZrxO3 (x = 0.00, 0.025, 0.05 and 0.075) compositions are investigated experimentally. Room temperature x-ray diffraction revealed change in phase from rhombohedral (R3c) to pseudocubic (Pm-3m) structure with Zr content. Substitution creates lattice disorder and compositional inhomogeneity was indentified in Raman spectra. Dielectric constant shows the depolarization temperature Td decreases with increasing Zr content. At x = 0.05, exhibit an improved P-E hysteresis and strong relaxor-ferroelectric behaviour near Td is clearly indicates the coexistence of polar and non-polar region in these ceramics.

Lattice, Charge, and Spin Phase Inhomogeneity in Complex-Striped Quantum Matter

The Superstripes 2016 conference, held on June 23-29, 2016 in the island of Ischia in Italy celebrated the 20th anniversary of this series of conferences. For 20 years structural, electronic, and magnetic phase inhomogeneities in quantum matter have been the scientific focus for a growing physics community interested in complexity in quantum matter. It has been the meeting point for different scientific communities facing the challenging project to unveil the complex space and time landscapes in quantum matter. The interesting spatial inhomogeneity length scale of multiple coexisting phase ranges from atomic to mesoscopic and the time fluctuations are spread over multiple time scales. The response of these materials changes using different experimental techniques with different spatial and time resolution probing different aspects of the quantum complexity.

Dynamic nonlinearity in epitaxialBaTiO3films

Dynamic dielectric and piezoelectric constants of ferroelectrics increase proportionally to the amplitude of alternating electric field as a result of hysteretic Rayleigh-type motion of domain walls. Here a hysteresis-free quadratic field dependence of the dynamic dielectric response is experimentally demonstrated in the absence of domain walls in epitaxial $\mathrm{BaTi}{\mathrm{O}}_{3}$ films. This extraordinary behavior is related to polar entities, whose presence is confirmed by the Vogel-Fulcher relaxation. The polar entities are ascribed to polarization fluctuations associated with lattice inhomogeneity.

Complex Lattice and Charge Inhomogeneity Favoring Quantum Coherence in High-Temperature Superconductors

The presence of two components in the electron fluid of high temperature superconductors and the complex charge and lattice inhomogeneity have been the hot topics of the international conference of the superstripes series, Superstripes 2015, held in Ischia in 2015. The debate on the mechanisms for reaching room temperature superconductivity has been boosted by the discovery of superconductivity with the highest critical temperature in pressurized sulfur hydride. Different complex electronic and structural landscapes showing up in superconductors which resist to the decoherence effects of high temperature has been discussed. While low temperature superconductors described by the BCS approximation are made of a single condensate in the weak coupling the high temperature superconductors are made of coexisting multiple condensates, in different spots of the k-space and the real space, some in the BCS-BEC crossover regime and others in the BCS regime. The role of shape resonance in the exchange interaction between these different condensates, like the Fano-Feshbach Resonance in ultracold gasses, is emerging as a key term for high temperature superconductivity.

Strain inhomogeneities in epitaxial BaFe2As2 thin films

Epitaxial BaFe2As2 thin films grown by pulsed laser deposition on spinel substrates with a thin iron buffer layer show strain‐induced superconductivity. Using high resolution electron backscatter diffraction in a scanning electron microscope very small orientation changes (≤ 0.2°) of the lattice and strain inhomogeneities on a length scale of few 100 nm or less were measured. Furthermore, partially strain relaxed areas were revealed. It was found, that the quality of the BaFe2As2 thin films crucially depends on the iron buffer layer.

Defect tolerance and the effect of structural inhomogeneity in plasmonic DNA-nanoparticle superlattices

Bottom-up assemblies of plasmonic nanoparticles exhibit unique optical effects such as tunable reflection, optical cavity modes, and tunable photonic resonances. Here, we compare detailed simulations with experiment to explore the effect of structural inhomogeneity on the optical response in DNA-gold nanoparticle superlattices. In particular, we explore the effect of background environment, nanoparticle polydispersity (>10%), and variation in nanoparticle placement (∼5%). At volume fractions less than 20% Au, the optical response is insensitive to particle size, defects, and inhomogeneity in the superlattice. At elevated volume fractions (20% and 25%), structures incorporating different sized nanoparticles (10-, 20-, and 40-nm diameter) each exhibit distinct far-field extinction and near-field properties. These optical properties are most pronounced in lattices with larger particles, which at fixed volume fraction have greater plasmonic coupling than those with smaller particles. Moreover, the incorporation of experimentally informed inhomogeneity leads to variation in far-field extinction and inconsistent electric-field intensities throughout the lattice, demonstrating that volume fraction is not sufficient to describe the optical properties of such structures. These data have important implications for understanding the role of particle and lattice inhomogeneity in determining the properties of plasmonic nanoparticle lattices with deliberately designed optical properties.

Irreversible thermodynamics of creep in crystalline solids

We develop an irreversible thermodynamics framework for the description of creep deformation in crystalline solids by mechanisms that involve vacancy diffusion and lattice site generation and annihilation. The material undergoing the creep deformation is treated as a non-hydrostatically stressed multi-component solid medium with non-conserved lattice sites and inhomogeneities handled by employing gradient thermodynamics. Phase fields describe microstructure evolution which gives rise to redistribution of vacancy sinks and sources in the material during the creep process. We derive a general expression for the entropy production rate and use it to identify of the relevant fluxes and driving forces and to formulate phenomenological relations among them taking into account symmetry properties of the material. As a simple application, we analyze a one-dimensional model of a bicrystal in which the grain boundary acts as a sink and source of vacancies. The kinetic equations of the model describe a creep deformation process accompanied by grain boundary migration and relative rigid translations of the grains. They also demonstrate the effect of grain boundary migration induced by a vacancy concentration gradient across the boundary.

Multiscale distribution of oxygen puddles in 1/8 doped YBa2Cu3O6.67

Despite intensive research a physical explanation of high Tc superconductors remains elusive. One reason for this is that these materials have generally a very complex structure making useless theoretical models for a homogeneous system. Little is known on the control of the critical temperature by the space disposition of defects because of lack of suitable experimental probes. X-ray diffraction and neutron scattering experiments used to investigate y oxygen dopants in YBa2Cu3O6+y lack of spatial resolution. Here we report the spatial imaging of dopants distribution inhomogeneity in YBa2Cu3O6.67 using scanning nano X-ray diffraction. By changing the X-ray beam size from 1 micron to 300 nm of diameter, the lattice inhomogeneity increases. The ordered oxygen puddles size distribution vary between 6–8 nm using 1 × 1 μm2 beam, while it is between 5–12 nm with a fat tail using the 300 × 300 nm2 beam. The increased inhomogeneity at the nanoscale points toward a network of superconducting puddles made of ordered oxygen interstitials.