Search

Magnetic interfaces and the phenomena arising from them drive both the design of modern spintronics and fundamental research. Recently, it was revealed that through designing magnetic frustration in configurationally complex entropy stabilized oxides, exchange bias can occur in structurally single crystal films. This eliminates the need for complex heterostructures and nanocomposites in the design and control of magnetic response phenomena. In this work, we demonstrate through hole doping of a high entropy perovskite oxide that tuning of magnetic responses can be achieved. With detailed magnetometry, we show magnetic coupling exhibiting a variety of magnetic responses including exchange bias and antiferromagnetic spin reversal in the entropy stabilized ABO3 perovskite oxide La1−xSrx(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 family. We find that manipulation of the A-site charge state can be used to balance magnetic phase compositions and coupling responses. This allows for the creation of highly tunable exchange bias responses. In the low Sr doping regime, a spin frustrated region arising at the antiferromagnetic phase boundary is shown to directly couple to the antiferromagnetic moments of the film and emerges as the dominant mechanism, leading to a vertical shift of magnetization loops in response to field biasing. At higher concentrations, direct coupling of antiferromagnetic and ferromagnetic regions is observed. This tunability of magnetic coupling is discussed within the context of these three competing magnetic phases, revealing critical features in designing exchange bias through exploiting spin frustration and disorder in high entropy oxides.

Botryosphaeria dothidea is a pathogenic fungus that can cause apple ring rot, a destructive apple disease in China. There have been reports on its molecular pathogenesis, but the pathogenic substances still remain unknown. In the present study, instrument analysis including UPLC-high-resolution mass spectrometry (HRMS) and nuclear magnetic resonance showed that B. dothidea fermentation broth contained (R)-(-)-mellein, a well-known fungal enantiomer of mellein. For further confirmation, a UPLC-MS/MS method for the determination of mellein was developed and validated. By this method, mellein was found to also exist in B. dothidea-infected apple fruits and branches with concentration ranges of 0.14-0.94 and 5.88-80.29 mg/kg, respectively. The concentration in fruits reached a peak at 48 h after pathogen inoculation, while a sustained concentration increase was achieved within 11 days for branches. Simultaneously, it was evident that there was a relation between disease spot expansion and mellein production kinetics in apple tissue. Phytotoxic bioassay showed that mellein could cause discoloration and death of apple leaves and browning in stems. Therefore, we confirmed that mellein was one of the pathogenic substances of B. dothidea. The present study provided additional data for the research on the pathogenesis of this pathogen.

Single crystalline BaMnSb2 is considered as a 3D Weyl semimetal with the 2D electronic structure containing Dirac cones from the Sb sheet. We report experimental investigation of low-temperature cleaved BaMnSb2 surfaces using scanning tunneling microscopy/spectroscopy and low energy electron diffraction. By natural cleavage, we find two terminations: one is Ba (above the orthorhombically distorted Sb sheet) and another Sb2 (at the surface of the Sb/Mn/Sb sandwich layer). Both terminations show the 2 × 1 surface reconstructions, with drastically different morphologies and electronic properties, however. The reconstructed structures, defect types and nature of the electronic structures of the two terminations are extensively studied. The quasiparticle interference (QPI) analysis is conducted at the energy range between −2 V and 2 V, although no interesting states are observed near the Fermi level, the surface-projected electronic band structures strongly depend on the surface termination above 1.6 V. The existence of defects can greatly modify the local density of states to create electronic phase separations on the surface in the order of tens of nm scale. Our observation on the atomic structures of the terminations and the corresponding electronic structures provides critical information towards an understanding of topological properties of BaMnSb2.

We report the magnetic and electronic transport properties of Mn-doped LaTi

We report nanoscale Eu0.5Ba0.5TiO3, a multiferroic in the bulk and candidate in the search to quantify the electric dipole moment of the electron. Eu0.5Ba0.5TiO3, in the form of nanoparticles and other nanostructures is interesting for nanocomposite integration, biomedical imaging and fundamental research, based upon the prospect of polarizability, f-orbital magnetism and tunable optical/radio luminescence. We developed a [non-hydrolytic]sol–[H2O-activated]gel route, derived from in-house metallic Ba(s)/Eu(s) alkoxide precursors and Ti{(OCH(CH3)2}4. Two distinct nanoscale compounds of Ba:Ti:Eu with the parent perovskite crystal structure were produced, with variable dielectric, magnetic and optical properties, based on altering the oxidizing/reducing conditions. Eu0.5Ba0.5TiO3 prepared under air/O2 atmospheres produced a spherical core–shell nanostructure (30–35 nm), with perovskite Eu0.5Ba0.5TiO3 nanocrystal core-insulating oxide shell layer (∼3 nm), presumed a pre-pyrochlore layer abundant with Eu3+. Fluorescence spectroscopy shows a high intensity 5D0 → 7F2 transition at 622 nm and strong red fluorescence. The core/shell structure demonstrated excellent capacitive properties: assembly into dielectric thin films gave low conductivity (2133 GΩ mm−1) and an extremely stable, low loss permittivity of eeff ∼25 over a wide frequency range (tan δ < 0.01, 100 kHz–2 MHz). Eu0.5Ba0.5TiO3 prepared under H2/argon produced more irregular shaped nanocrystals (20–25) nm, with a thin film permittivity around 4 times greater (eeff 101, tan δ < 0.05, 10 kHz–2 MHz, σ ∼59.54 kΩ mm−1). Field-cooled magnetization values of 0.025 emu g−1 for EBTO-Air and 0.84 emu g−1 for EBTO-Argon were observed. X-ray photoelectron spectroscopy analysis reveals a complex interplay of EuII/III/TiIII/IV configurations which contribute to the observed ferroic and fluorescence behavior.

Atomically thin two-dimensional (2D) metals may be key ingredients in next-generation quantum and optoelectronic devices. However, 2D metals must be stabilized against environmental degradation and integrated into heterostructure devices at the wafer scale. The high-energy interface between silicon carbide and epitaxial graphene provides an intriguing framework for stabilizing a diverse range of 2D metals. Here we demonstrate large-area, environmentally stable, single-crystal 2D gallium, indium and tin that are stabilized at the interface of epitaxial graphene and silicon carbide. The 2D metals are covalently bonded to SiC below but present a non-bonded interface to the graphene overlayer; that is, they are 'half van der Waals' metals with strong internal gradients in bonding character. These non-centrosymmetric 2D metals offer compelling opportunities for superconducting devices, topological phenomena and advanced optoelectronic properties. For example, the reported 2D Ga is a superconductor that combines six strongly coupled Ga-derived electron pockets with a large nearly free-electron Fermi surface that closely approaches the Dirac points of the graphene overlayer.

BaMn3Ti4O14+δ (δ = 0.25, BMT-134), a recently discovered single-phase multiferroic complex oxide was doped with varying concentrations of Fe in order to assess the effect on magnetic and dielectric behavior. The novel compound BaMn3−xFexTi4O14+δ (BMFT) was prepared via a sol–gel chemical solution processing method. Four substituted variations were synthesized: BaMn3−xFexTi4O14+δ (BMFT) with x = 1, 1.5, 2, and 2.25. The approach afforded a nanocrystalline product, with control over structure and morphology, while successfully allowing increasing amounts of iron to be incorporated into the structure. All variants belong to the same hollandite I4/m crystal class as the parent compound, confirmed by powder XRD. Electron microscopy (TEM, EDS and SEM) provided characterization of the microstructure and elemental composition. Mossbauer spectroscopy was used to probe the local chemical environment of Fe present within the nanocrystals, to indicate oxidation state and bonding geometry. The BMFT material system was characterized as a function of temperature and applied magnetic field: M–T and M–H curves were obtained (by MPMS) and allowed the determination of Curie/Weiss constants through fitting and low temperature hysteresis respectively. The Weiss constant becomes increasingly positive as Fe is added until an observed inflection point, indicative of an antiferromagnetic to paramagnetic short-range interaction transition. The frequency dependent dielectric permittivity of the series of BMFT compounds with differing Fe concentration, was obtained on MIM structures prepared from pressed pellets with a nanostructured morphology. The results show how Fe concentration can strongly influence dielectric behavior. Dielectric constants ranging from 100–1600 (low frequencies) to 150–200 (high frequencies) were observed, together with a decrease in the AC conductivity with increasing Fe.

Precise control of lattice mismatch accommodation and interfacial cation diffusion is critical to modulate correlated functionalities in epitaxial heterostructures, particularly when the interface composition is positioned near a compositional phase transition boundary. Here we select La1−xSrxMnO3 (LSMO) as a prototype phase transition oxide and establish vertical epitaxial interfaces with NiO for exploring the strong interplay between strain accommodation, stoichiometry modification, and localized electron transport across the interface. It is found that localized stoichiometry modification overcomes the dead layer problem plaguing LSMO and leads to strongly directional conductivity, as manifested by a more than three orders of magnitude difference between out-of-plane and in-plane conductivity. Comprehensive atomic scale structural characterization and transport measurements reveal that this emerging behavior is created by a compositional change produced by preferential cation diffusion that pushes the LSMO phase transition from insulating into metallic within an ultrathin interface region. This study explores the nature of unusual electrical conductivity at vertical epitaxial interfaces and highlights the beneficial role of controllable cation diffusion that enables emerging functionalities for a broad range of potential applications such as memristors, spintronic devices, and novel nanoelectronic devices using strongly correlated materials.

The atomic and electronic structures of pristine PdSe2 as well as various intrinsic vacancy defects in PdSe2 are studied comprehensively by combining scanning tunneling microscopy, spectroscopy, an...

We report the magnetic and electronic transport properties of Mn-doped LaTi1−x Mn x O3 (x= 0, 0.1, 0.3, 0.5) as a function of temperature and an applied magnetic field. It was found that the Mn-doped samples show a magnetic transition which is not present in the parent LaTiO3. The Mn-doped samples showed fluctuations in magnetization at low fields below their Néel transition temperature indicating electronic phase separation in the material. Increased Mn content in the sample strengthens the ferromagnetic-like moment while maintaining G-type antiferromagnetic phase by charge transfer from Mn to Ti and influencing orbital ordering of the Ti3+ t2g orbitals. The results are discussed in parallel with transport and bulk magnetization measurements detailing the electronic behavior. An additional context for the mechanism is supported by first-principles density-function theory calculations.

The influence of hole doping on magnetic properties is mapped for the compositionally complex high-entropy oxide ${AB\mathrm{O}}_{3}$ perovskite ${\mathrm{La}}_{1\text{\ensuremath{-}}x}{\mathrm{Sr}}_{x}({\mathrm{Cr}}_{0.2}{\mathrm{Mn}}_{0.2}{\mathrm{Fe}}_{0.2}{\mathrm{Co}}_{0.2}{\mathrm{Ni}}_{0.2}){\mathrm{O}}_{3}$ $(0\ensuremath{\le}x\ensuremath{\le}0.5)$. It is found that aliovalent A-site substitution is a viable means to manipulate the magnetically active B-site sublattice. A series of single-crystal films are synthesized and show a general trend toward stronger ferromagnetic response and a shift in magnetic anisotropy as the Sr concentration increases. Magnetometry demonstrates complex and nonuniform responses similar to rigid and uncoupled composites at intermediate dopings. This behavior points to the presence of locally inhomogeneous magnetic phase competition, where ferromagnetic and antiferromagnetic magnetic contributions create a frustrated matrix containing uncompensated spins at the boundaries between these regions. The observations are discussed in the context of known responses to hole doping in the less complex ternary $\mathrm{La}{T}_{M}{\mathrm{O}}_{3}$ $({T}_{M}=\mathrm{Cr},\mathrm{Mn},\mathrm{Fe},\mathrm{Co},\mathrm{Ni})$ oxides, and they are found to be different from a simple sum of the doped parents. The results are summarized in a preliminary magnetic phase diagram.

The adatom arrays on surfaces offer an ideal playground to explore the mechanisms of chemical bonding via changes in the local electronic tunneling spectra. While this information is readily available in hyperspectral scanning tunneling spectroscopy data, its analysis has been considerably impeded by a lack of suitable analytical tools. Here we develop a machine learning based workflow combining supervised feature identification in the spatial domain and unsupervised clustering in the energy domain to reveal the details of structure-dependent changes of the electronic structure in adatom arrays on the Co3Sn2S2 cleaved surface. This approach, in combination with first-principles calculations, provides insight for using artificial neural networks to detect adatoms and classifies each based on their local neighborhood comprised of other adatoms. These structurally classified adatoms are further spectrally deconvolved. The unexpected inhomogeneity of electronic structures among adatoms in similar configurations is unveiled using this method, suggesting there is not a single atomic species of adatoms, but rather multiple types of adatoms on the Co3Sn2S2 surface. This is further supported by a slight contrast difference in the images (or slight size variation) of the topography of the adatoms.

Atomic structures and adatom geometries of surfaces encode information about the thermodynamics and kinetics of the processes that lead to their formation, and which can be captured by a generative physical model. Here we develop a workflow based on a machine-learning-based analysis of scanning tunneling microscopy images to reconstruct the atomic and adatom positions, and a Bayesian optimization procedure to minimize statistical distance between the chosen physical models and experimental observations. We optimize the parameters of a 2- and 3-parameter Ising model describing surface ordering and use the derived generative model to make predictions across the parameter space. For concentration dependence, we compare the predicted morphologies at different adatom concentrations with the dissimilar regions on the sample surfaces that serendipitously had different adatom concentrations. The proposed workflow can be used to reconstruct the thermodynamic models and associated uncertainties from the experimental observations of materials microstructures. The code used in the manuscript is available at https://github.com/saimani5/Adatom_interactions.

Ba(Ti,Fe)O3 is a useful system for the exploration of multiferroic properties as a function of composition and variation in structure, based upon a model of intersubstitution of the B site cation. ...

We report nanoscale Eu

Magnetic insulators are important materials for a range of next-generation memory and spintronic applications. Structural constraints in this class of devices generally require a clean heterointerface that allows effective magnetic coupling between the insulating layer and the conducting layer. However, there are relatively few examples of magnetic insulators that can be synthesized with surface qualities that would allow these smooth interfaces and precisely tuned interfacial magnetic exchange coupling, which might be applicable at room temperature. In this work, we demonstrate an example of how the configurational complexity in the magnetic insulator layer can be used to realize these properties. The entropy-assisted synthesis is used to create single-crystal (Mg

Quantum materials are usually heterogeneous, with structural defects, impurities, surfaces, edges, interfaces, and disorder. These heterogeneities are sometimes viewed as liabilities within conventional systems; however, their electronic and magnetic structures often define and affect the quantum phenomena such as coherence, interaction, entanglement, and topological effects in the host system. Therefore, a critical need is to understand the roles of heterogeneities in order to endow materials with new quantum functions for energy and quantum information science applications. In this article, several representative examples are reviewed on the recent progress in connecting the heterogeneities to the quantum behaviors of real materials. Specifically, three intertwined topic areas are assessed: i) Reveal the structural, electronic, magnetic, vibrational, and optical degrees of freedom of heterogeneities. ii) Understand the effect of heterogeneities on the behaviors of quantum states in host material systems. iii) Control heterogeneities for new quantum functions. This progress is achieved by establishing the atomistic-level structure-property relationships associated with heterogeneities in quantum materials. The understanding of the interactions between electronic, magnetic, photonic, and vibrational states of heterogeneities enables the design of new quantum materials, including topological matter and quantum light emitters based on heterogenous 2D materials.

The interplay between magnetism and nontrivial topology in magnetic topological insulators (MTIs) is expected to give rise to exotic topological quantum phenomena like the quantum anomalous Hall effect and the topological axion states. A key to assessing these novel properties is to realize gapped topological surface sates. $\mathrm{Mn}{\mathrm{Bi}}_{2}{\mathrm{Te}}_{4}$ possesses nontrivial band topology with an intrinsic antiferromagnetic state. However, the highly electron-doped nature of the $\mathrm{Mn}{\mathrm{Bi}}_{2}{\mathrm{Te}}_{4}$ crystals obstructs the exhibition of the surface band gap. Here, we tailor the material through Sb substitution to reveal the gapped surface states in $\mathrm{Mn}{\mathrm{Bi}}_{2\text{\ensuremath{-}}x}{\mathrm{Sb}}_{x}{\mathrm{Te}}_{4}$. By shifting the Fermi level into the bulk band gap, we access the surface states and show a band gap of 50 meV at the Dirac point from quasiparticle interference measured by scanning tunneling microscopy (STM). Surface-dominant conduction is confirmed through transport spectroscopy measured by multiprobe STM below the N\'eel temperature. The surface band gap is robust against the out-of-plane magnetic field despite the promotion of field-induced ferromagnetism. The realization of bulk-insulating MTIs with the large exchange gap offers a promising platform for exploring emergent topological phenomena.

Multifunctional hybrid nanoparticles (NPs, ∼100 nm) that combine magnetic Fe3O4 nanocrystals and fluorescent carbon dots (CDs) in porous carbon (C) were successfully synthesized using a one-pot solvothermal method by simply increasing the H2O2 concentration. The resultant Fe3O4@C-CDs hybrid NPs not only demonstrate excellent magnetic responsive properties (Ms = 32.5 emu g−1) and magnetic resonance imaging ability (r*2 = 674.4 mM−1 s−1) from the Fe3O4 nanocrystal core, but also exhibit intriguing photoluminescent (quantum yield ∼6.8%) properties including upconversion fluorescence and excellent photostability from the CDs produced in the porous carbon. The hybrid NPs can enter the intracellular region and illuminate mouse melanoma B16F10 cells under different excitation wavelengths. Meanwhile, the mesoporous carbon shell and hydrophilic surface functional groups endow the hybrid NPs with high loading capacity (835 mg g−1) for the anti-cancer drug doxorubicin and excellent stability in aqueous solutions. More importantly, the hybrid NPs can absorb and convert near-infrared (NIR) light to heat due to the existence of CDs, and thus, can realise NIR-controlled drug release and combined photothermo/chemotherapy for high therapeutic efficacy. Such nanostructured Fe3O4@C-CDs hybrid NPs demonstrate great promise towards advanced nanoplatforms for simultaneous imaging diagnostics and high efficacy therapy.

A class of multifunctional hybrid nanoparticles (NPs) that can integrate a magnetic core, silver (Ag) nanocrystals, and a biocompatible poly(ethylene glycol) (PEG) shell were synthesized and characterized and their applications as antibacterial agents, optical labels for cellular imaging and drug carriers were tested. The synthetic strategy involves a one-step solvothermal synthesis of Fe

It is noteworthy that chemical substitution of BaFe

Configurational disorder can have a dominating role in the formation of macroscopic functional responses in strongly correlated materials. Here, we use entropy-stabilization synthesis to create single-crystal epitaxial $\mathrm{AB}{\mathrm{O}}_{3}$ perovskite thin films with equal atomic concentration of 3d transition-metal cations on the B-site sublattice. X-ray diffraction, atomic force microscopy, and scanning transmission electron microscopy of $\mathrm{La}(\mathrm{C}{\mathrm{r}}_{0.2}\mathrm{M}{\mathrm{n}}_{0.2}\mathrm{F}{\mathrm{e}}_{0.2}\mathrm{C}{\mathrm{o}}_{0.2}\mathrm{N}{\mathrm{i}}_{0.2}){\mathrm{O}}_{3}$ (L5BO) films demonstrate excellent crystallinity, smooth film surfaces, and uniform mixing of the 3d transition-metal cations throughout the B-site sublattice. The magnetic properties are strongly dependent on substrate-induced lattice anisotropy and suggest the presence of long-range magnetic order in these exceptionally disordered materials. The ability to populate multiple elements onto a single sublattice in complex crystal structures opens new possibilities to design functionality in correlated systems and enable novel fundamental studies seeking to understand how diverse local bonding environments can work to generate macroscopic responses, such as those driven by electron-phonon channels and complex exchange interaction pathways.

${\mathrm{Fe}}_{3\ensuremath{-}x}{\mathrm{GeTe}}_{2}$ is a layered van der Waals magnetic material with a relatively high ordering temperature and large anisotropy. While most studies have concluded the interlayer ordering to be ferromagnetic, there have also been reports of interlayer antiferromagnetism in ${\mathrm{Fe}}_{3\ensuremath{-}x}{\mathrm{GeTe}}_{2}$. Here, we investigate the interlayer magnetic ordering by neutron diffraction experiments, scanning tunneling microscopy (STM) and spin-polarized STM measurements, density functional theory plus U calculations, and STM simulations. We conclude that the layers of ${\mathrm{Fe}}_{3\ensuremath{-}x}{\mathrm{GeTe}}_{2}$ are coupled ferromagnetically and that in order to capture the magnetic and electronic properties of ${\mathrm{Fe}}_{3\ensuremath{-}x}{\mathrm{GeTe}}_{2}$ within density functional theory, Hubbard U corrections need to be taken into account.

The manipulation of mesoscale domain wall phenomena has emerged as a powerful strategy for designing ferroelectric responses in functional devices, but its full potential is not yet realized in the field of magnetism. This work shows a direct connection between magnetic response functions in mechanically strained samples of Mn3O4 and MnV2O4 and stripe‐like patternings of the bulk magnetization which appear below known magnetostructural transitions. Building off previous magnetic force microscopy data, a small‐angle neutron scattering is used to show that these patterns represent distinctive magnetic phenomena which extend throughout the bulk of two separate materials, and further are controllable via applied magnetic field and mechanical stress. These results are unambiguously connected to the anomalously large magnetoelastic and magnetodielectric response functions reported for these materials, by performing susceptibility measurements on the same crystals and directly correlating local and macroscopic data., Magnetostructural transitions in the ferrimagnetic spinels Mn3O4 and MnV2O4 are linked to increased spin–lattice coupling, from which novel magnetic domain structures emerge on the mesoscale. Small‐angle neutron scattering measures the response of these domain patterns to applied magnetic field and stress. Correlations between scattering and bulk probes demonstrate tuning of macroscopic response functions via alterations to the domain structure.

The atomic and electronic structures of pristine PdSe

This study investigates the changes of magnetic ordering temperature via nano- and mesoscale structural features in an iron arsenide. Although magnetic ground states in quantum materials can be theoretically predicted from known crystal structures and chemical compositions, the ordering temperature is harder to pinpoint due to such local lattice variations. In this work we find surprisingly that a locally disordered material can exhibit a significantly larger Neel temperature (TN) than an ordered material of precisely the same chemical stoichiometry. Here, a EuFe2As2 crystal, which is a 122 parent of iron arsenide superconductors, is found through synthesis to have ordering below TN = 195 K (for the disordered crystal) or TN = 175 K (for the ordered crystal). In the higher TN crystals, there are shorter planar Fe-Fe bonds [2.7692(2) A vs. 2.7745(3) A], a randomized in-plane defect structure, and diffuse scattering along the [00L] crystallographic direction that manifests as a rather broad specific heat peak. For the lower TN crystals, the a-lattice parameter is larger and the in-plane microscopic structure shows defect ordering along the antiphase boundaries, giving a larger TN and a higher superconducting temperature (Tc) upon the application of pressure. First principles calculations find a strong interaction between c-axis strain and interlayer magnetic coupling, but little impact of planar strain on the magnetic order. Neutron single-crystal diffraction shows that the low-temperature magnetic phase transition due to localized Eu moments is not lattice or disorder sensitive, unlike the higher-temperature Fe sublattice ordering. This study demonstrates a higher magnetic ordering point arising from local disorder in 122., 4 main figures

Thin flakes of Cr1/3NbS2 are fabricated successfully via microexfoliation techniques. Temperature-dependent and field-dependent magnetizations of thin flakes with various thicknesses are investigat...

In this paper, the effect of non-collimated light path on moire deflectometry is studied based on scalar diffraction theory. The complex amplitude of non-collimated light path is initially deduced, which shows it has a magnification factor compared with that of the collimated light path. Then, the intensity distribution and fringe equation are obtained, analyzed and discussed under different orders filtering. Based on which, it is found that a series of linear function under non-collimated light without phase object causes the moire fringes to tilt, and the effect of phase object's position on final moire fringe is compared. Finally, the relevant theoretical derivation results are validated by comparing with that of experiment, which proves our theoretical deduction is reasonable. In conclusion, the results could provide some references for expanding the application range of moire deflectometry.

Interface plays a critical role in determining the physical properties and device performance of heterostructures. Traditionally, lattice mismatch, resulting from the different lattice constants of the heterostructure, can induce epitaxial strain. Over past decades, strain engineering has been demonstrated as a useful strategy to manipulate the functionalities of the interface. However, mismatch of crystal symmetry at the interface is relatively less studied due to the difficulty of atomically structural characterization, particularly for the epitaxy of low symmetry correlated materials on the high symmetry substrates. Overlooking those phenomena restrict the understanding of the intrinsic properties of the as- determined heterostructure, resulting in some long-standing debates including the origin of magnetic and ferroelectric dead layers. Here, perovskite LaCoO3-SrTiO3 superlattice (SL) is used as a model system to show that the crystal symmetry effect can be isolated by the existing interface strain. Combining the state-of-art diffraction and electron microscopy, it is found that the symmetry mismatch of LaCoO3-SrTiO3 SL can be tuned by manipulating the SrTiO3 layer thickness to artificially control the magnetic properties. The work suggests that crystal symmetry mismatch can also be designed and engineered to act as an effective strategy to generate functional properties of perovskite oxides.

Results of DC magnetization and x-ray diffraction measurements under hydrostatic pressure are reported for the CdCr2S4 spinel compound. Magnetization measurements were performed in a polycrystalline sample up to 14 kbar in the 20–220 K temperature range. At low applied magnetic fields an anomalous susceptibility behavior, associated to magnetic clusters, persists up to 14 kbar. X-ray synchrotron diffraction spectra acquired under pressure show a strong linear correlation between the variation of lattice parameters under pressure and the variation of the Cr–Cr distance. In contrast, the S-Cr-S angles remain constant. Clearly, the CdCr2S4 magnetic properties are strongly sensitive to pressure variations and the Cr local distortions observed in this compound promote a competition between direct antiferromagnetic and super-exchange ferromagnetic interactions within such short-range magnetic clusters.

Ferromagnetic insulators are rather rare but possess great technological potential in, for example, spintronics. Individual control of ferromagnetic properties and electronic transport provides a useful design concept of multifunctional oxide heterostructures. We studied the close correlation among the magnetism, atomic structure, and electronic structure of oxide heterostructures composed of the ferromagnetic perovskite LaCoO3 and the antiferromagnetic brownmillerite SrCoO2.5 epitaxial thin film layers. By reversing the stacking sequence of the two layers, we could individually modify the electric resistance and saturation magnetic moment. The ferromagnetic insulating behavior in the heterostructures was understood in terms of the electronic reconstruction at the oxide surface/interfaces and crystalline quality of the constituent layers.

Combined scanning tunneling microscopy, spectroscopy and local barrier height (LBH) studies show that low-temperature-cleaved optimally-doped Ba(Fe1-xCox)2As2 crystals with x=0.06, with Tc = 22 K, have complicated morphologies. Although the cleavage surface and hence the morphologies are variable, the superconducting gap maps show the same gap widths and nanometer size inhomogeneities irrelevant to the morphology. Based on the spectroscopy and LBH maps, the bright patches and dark stripes in the morphologies are identified as Ba and As dominated surface terminations, respectively. Magnetic impurities, possibly due to cobalt or Fe atoms, are believed to create local in-gap state and in addition suppress the superconducting coherence peaks. This study will clarify the confusion on the cleavage surface terminations of the Fe-based superconductors, and its relation with the electronic structures., Accepted to Nano Letters (5 figures)

We investigate the chemical substitution of group 5 into BaFe2As2 (122) iron arsenide, in the effort to understand why Fe-site hole doping of this compound (e.g., using group 5 or 6) does not yield bulk superconductivity. We find an increase in c-lattice parameter of the BaFe2As2 with the substitution of V, Nb, or Ta; the reduction in c predicts the lack of bulk superconductivity [1] that is confirmed here through transport and magnetization results. However, our spectroscopy measurements find a coexistence of antiferromagnetic and local superconducting nanoscale regions in V-122, observed for the first time in a transition-metal hole-doped iron arsenide. In BaFe2As2, there is a complex connection between local parameters such as composition and lattice strain, average lattice details, and the emergence of bulk quantum states such as superconductivity and magnetism. [1] L. M. N. Konzen, and A. S. Sefat, J. Phys.: Condens. Matter 29 (2017), 083001., Comment: 5 figures (including supplemental)

Ferromagnetic insulators have great potential for spintronic applications. For such applications, it is essential to find materials with a robust and controllable ferromagnetic insulating phase. However, because ferromagnetism in functional transition-metal oxides is usually coupled to metallicity, ferromagnetic insulators are very rare and independent control of their magnetic and electrical properties is difficult. In this study, the electrical, magnetic, and optical properties of ${(\mathrm{LaCo}{\mathrm{O}}_{3})}_{n}/{(\mathrm{SrCo}{\mathrm{O}}_{2.5})}_{n}$ superlattice films are investigated for the manipulation of the ferromagnetic insulating phase. While the superlattices remain insulating irrespective of the periodicity $n$, the electronic structure and magnetic state vary drastically. Superlattices with large periodicities $n$ of 10 and 20 show a ferromagnetic transition at a critical temperature ${T}_{\mathrm{C}}$ of $\ensuremath{\sim}80\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. With decreasing periodicity and increasing interface density of the superlattices, system with $n=4$ becomes almost nonmagnetic, while in systems with $n=2$ and 1, a reentrant ferromagnetic phase is observed at ${T}_{\mathrm{C}}$ of $\ensuremath{\sim}180$ and $\ensuremath{\sim}225\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, respectively. Optical spectroscopy reveals that the fine control of the magnetic ground state is achieved by the modified electronic structure associated with the spin-state transition. Our results suggest an important design principle to create and manipulate the ferromagnetic insulating properties of Co-based oxide thin films.

Characterization of the onset of a phase transition is often challenging due to the fluctuations of the correlation length scales of the order parameters. This is especially true for second-order structural-phase transition due to minute changes involved in the relevant lattice constants. A classic example is the cubic-to-tetragonal second-order phase transition in SrTiO(3) (STO), which is so subtle that it is still unresolved. Here, we demonstrate an approach to resolve this issue by epitaxially grown rhombohedral La(0.7)Sr(0.3)MnO(3) (LSMO) thin films on the cubic STO (100) substrate. The shear strain induced nanotwinning waves in the LSMO film are extremely sensitive to the cubic-to-tetragonal structural-phase transitions of the STO substrate. Upon cooling from room temperature, the development of the nanotwinning waves is spatially inhomogeneous. Untwinned, atomically flat domains, ranging in size from 100 to 300 nm, start to appear randomly in the twinned phase between 265 and 175 K. At ∼139 K, the untwinned, atomically flat domains start to grow rapidly into micrometer scale and finally become dominant at ∼108 K. These results indicate that the low-temperature tetragonal precursor phase of STO has already nucleated at 265 K, significantly higher than the critical temperature of STO (∼105 K). Our work paves a pathway to visualize the onset stages of structural-phase transitions that are too subtle to be observed using direct-imaging methods.

The electronic structure inhomogeneities in Co, Ni, and Cr doped BaFe2As2 122 single crystals are compared using scanning tunneling microscopy/spectroscopy (STM/S) at the nanoscale within three bulk property regions in the phase diagram: a pure superconducting (SC) dome region (Co-122), a coexisting SC and antiferromagnetic (AFM) region (Ni-122), and a non-SC region (Cr-122). Machine learning is utilized to categorize the various nanometer scale inhomogeneous electronic states, described here as in-gap, L-shape and S-shape states immersed into the SC matrix for Ni-and Co-doped 122, and L-shape and S-shape states into the metallic matrix for Cr-doped 122. Although the relative percentages of in-gap, L-shape and S-shape states vary in the three samples, the total volume fraction of the three electronic states is quite similar. This is coincident with the number of electrons (Ni0.04 and Co0.08) and holes (Cr0.04) doped into the 122 compound. By combining the volume fractions of the three states, the local density of states (LDOS), magnetic field dependent behavior and global properties in these three samples, the in-gap state is confirmed as a magnetic impurity state from the Co or Ni dopants. In addition, the L-shape state is identified as a spin density wave (SDW) which competes with the SC phase, and the S-shape state is found to be another form of magnetic order which constructively cooperates with the SC phase, rather than competing with it. The comparison of the vortex structures indicates that the inhomogeneous electronic states serve as pinning centers for stabilizing the vortex lattice.

We numerically demonstrate that a properly designed guided mode resonance filter (GMRF) with suspended silica (SiO2) subwavelength grating (SSG) can exhibit non-polarizing resonant filtering effect under normal incidence. By choosing appropriate parameters, including the incident wavelength, the grating period, the grating thickness, and the fill factor, the same resonance wavelengths for both transverse electric (TE) and transverse magnetic (TM) polarizations can be achieved. Results show that high reflection (more than 99.9%) can be obtained at the resonance wavelength (1.55 μm), and the full-width at half maximums (FWHMs) of TE- and TM-polarized light are only 1.0 × 10−2 μm and 1.4 × 10−3 μm, respectively. The reflectance peak splits into two branches when the incident light deviates from normal incidence. It is expected that the designed SSG should have applications in optical telecommunication systems or wavelength division multiplexing systems with an arbitrary state of polarization.

Finite range ferromagnetism and antiferromagnetism in two-dimensional (2D) systems within an isotropic Heisenberg model at non-zero temperature were originally proposed to be impossible. However, recent theoretical studies using an Ising model have shown that 2D magnetic crystals can exhibit magnetism. Experimental verification of existing 2D magnetic crystals in this system has remained exploratory. In this work we exfoliated CrSiTe3, a bulk ferromagnetic semiconductor, to mono- and few-layer 2D crystals onto a Si/SiO2 substrate. Raman spectra indicate good stability and high quality of the exfoliated flakes, consistent with the computed phonon spectra of 2D CrSiTe3, giving strong evidence for the existence of 2D CrSiTe3 crystals. When the thickness of the CrSiTe3 crystals is reduced to a few layers, we observed a clear change in resistivity at 80–120 K, consistent with theoretical calculations of the Curie temperature (Tc) of ∼80 K for the magnetic ordering of 2D CrSiTe3 crystals. The ferromagnetic mono- and few-layer 2D CrSiTe3 indicated here should enable numerous applications in nano-spintronics.

Manganese tetraphenylporphyrin bromide and iodide Mn(TPP)X (X = Br, 2; I, 3; TPP2− = meso-tetraphenylporphyrinate) are synthetic analogs of Mn(III) geoporphyrins. Crystal structures of 2 and 3 with chloroform in the lattices, Mn(TPP)Br·CHCl3 (2·CHCl3), Mn(TPP)I·CHCl3 (3·CHCl3), Mn(TPP)I·CDCl3 (3·CDCl3 in a different space group from 3·CHCl3), Mn(TPP)I·1.5CHCl3 (3·1.5CHCl3), and 2 with dichloromethane in the lattice, Mn(TPP)Br·CH2Cl2 (2·CH2Cl2), have been determined by single-crystal X-ray diffraction at 100 K or 298 K. Hirshfeld surface analyses of the crystal structures of 2·CHCl3, 2·CH2Cl2, 3·CHCl3, 3·CDCl3 and 3·1.5CHCl3 have been performed. Surprisingly the Mn(III)–Br and Mn(III)–I bonds in Mn(TPP)X (2–3) are about 0.2 A (8%) longer than Fe(III)–Br and Fe(III)–I bonds in S = 5/2 Fe(TPP)X (X = Br, 4; I, 5), although both Mn(III) and Fe(III) ions have the same radii. Magnetic properties of 2 and 3 have been studied by direct current (DC) and alternating current (AC) susceptibility measurements, high-field electron paramagnetic resonance (HFEPR), and inelastic neutron scattering (INS). With four unpaired electrons in Mn(TPP)X (X = Br, 2; I, 3), the bromide complex 2 in 2·CDCl3 possesses easy-axis anisotropy, as does the chloride analog Mn(TPP)Cl (1), with the axial (D) and rhombic (E) zero-field splitting parameters of D = –1.091(3) cm−1 and |E| = 0.087(2) cm−1. The iodide complex 3 in 3·CDCl3 becomes easy-plane with D = +1.30(1) cm−1 and |E| = 0.010(5) cm−1. Axial ZFS parameters D change from −2.290(5) cm−1 in 1, reported earlier, to −1.091(3) cm−1 in 2 and +1.30(1) cm−1 in 3.

It is noteworthy that chemical substitution of BaFe2As2 (122) with the noble elements Cu and Au gives superconductivity with a maximum T c ≈ 3 K, while Ag substitution (Ag-122) stays antiferromagnetic. For Ba(Fe1-x TM x )2As2, TM = Cu, Au, or Ag, and by doping an amount of x = 0.04, a-lattice parameter slightly increases (0.4%) for all TM dopants, while c-lattice decreases (-0.2%) for TM = Cu, barely moves (0.05%) for Au, and increases (0.2%) for Ag. Despite the naive expectation that the noble elements of group 11 should affect the quantum properties of 122 similarly, they produce significant differences extending to the character of the ground state. For the Ag-122 crystal, evidence of only a filamentary superconductivity is noted with pressure. However, for Au and Cu doping (x ≈ 0.03) we find a substantial improvement in the superconductivity, with T c increasing to 7 K and 7.5 K, respectively, under 20 kbar of pressure. As with the ambient pressure results, the identity of the dopant therefore has a substantial impact on the ground state properties. Density functional theory calculations corroborate these results and find evidence of strong electronic scattering for Au and Ag dopants, while Cu is comparatively less disruptive to the 122 electronic structure.