Electronic,Magnetic and Photocatalytic Properties in(Fe,Ni)-Codoped SrTiO3 with and without Oxygen Vacancies:a First-principles Study

The enhanced magnetic and photocatalytic properties of（Fe, Ni）-codoped SrTiO3 with and without oxygen vacancies are investigated using the first-principles calculations based on the density functional theory plus U calculations. It is revealed that the structure phase transition associated with O vacancy imposes significant influence on magnetic and optical properties. The results show that the Ni oxidation state in（Fe, Ni）-codoped SrTiO3 is about 2＋, which is different from that of 4＋ in Ni monodoped SrTiO3 in previous experimental investigations. The presence of O vacancy leads to a semiconductor-half-metal transition in codoped SrTiO3. The（Fe, Ni）-codoped SrTiO3 without O vacancy produces an enhanced magnetization and induces a giant magnetic moment of 3 μB, while a relatively small magnetic moment of 0.36 μB is generated in（Fe, Ni）-codoped SrTiO3 with O vacancy. The origin of the large enhancement of magnetic moment in（Fe, Ni）-codoped SrTiO3 without O vacancy was ascribed to the reduced hybridization in Fe–O bonds and the enhanced hybridization in Ni–O bonds, which modulated antiferromagnetic spin structure. The dispersion of the conduction bands and valence bands of codoped SrTiO3 is enhanced after codoping, which benefits the photocatalytic performance. Furthermore, the（Fe, Ni）-codoped SrTiO3 shows a remarkable red-shift of absorption spectra edge and induces a strong optical absorption in the visible light region, indicating that it could be taken as a potential candidate for photocatalytic materials.

Structural and electronic properties of Fe-doped BaTiO3 and SrTiO3

We have performed first principles calculations of Fe-doped BaTiO3 and SrTiO3. Dopant formation energy, structure distortion, band structure and density of states have been computed. The dopant formation energy is found to be 6.8eV and 6.5eV for Fe-doped BaTiO3 and SrTiO3 respectively. The distances between Fe impurity and its nearest O atoms and between Fe atom and Ba or Sr atoms are smaller than those of the corresponding undoped bulk systems. The Fe defect energy band is obtained, which mainly originates from Fe 3d electrons. The band gap is still an indirect one after Fe doping for both BaTiO3 and SrWiO3, but the gap changes from Γ-R point to Γ-X point.

First-principles study of electronic structure and magnetic properties of SrTi1-xMxO3 （M = Cr, Mn, Fe, Co, or Ni）

We used first-principles calculations to conduct a comparative study of the structure and the electronic and magnetic properties of SrTiO3 doped with a transition metal（TM）, namely, Cr, Mn, Fe, Co, or Ni. The calculated formation energies indicate that compared with Sr, Ti can be substituted more easily by the TM ions. The band structures show that SrTi0.875Cr0.125O3 and SrTi0.875Co0.125O3 are half metals, SrTio.sTDFe0.125O3 is a metal, and SrTi0.875Mn0.125O3 is a semiconductor. The 3d TM-doped SrTiO3 exhibits various magnetic properties, ranging from ferromagnetism （Cr-, Fe-, and Co-doped SrTiO3） to antiferromagnetism （Mn-doped SrTiO3） and nonmagnetism （Ni-doped SrTiO3）. The total magnetic moments are 4.0#8, 6.23μ8, and 2.0μ8 for SrTi0.75Cr0.25O3, SrTi0.75Fe0.25O3, and SrTi0.75Co0.25O3, respectively. Room-temperature ferromagnetism can be expected in Cr-, Fe-, and Co-doped SrTiO3, which agrees with the experimental observations. The electronic structure calculations show that the spin polarizations of the 3d states of the TM atoms are responsible for the ferromagnetism in these compounds. The magnetism of TM-doped SrTiO3 is explained by the hybridization between the TM-3d states and the O-2p states.

First-principles study of electronic structure and magnetic properties of Sr_(3)Fe_(2)O_(5) oxide

We investigate the electronic structure and magnetic properties of layered compound Sr_(3)Fe_(2)O_(5) based on firstprinciples calculations in the framework of density functional theory with GGA+U method.Under high pressure,the ladder-type layered structure of Sr_(3)Fe_(2)O_(5) is transformed into the infinite layered structure accompanied by a transition from G-type anti-ferromagnetic(AFM)insulator to ferromagnetic(FM)metal and a spin transition from S=2 to S=1.We reproduce these transformations in our calculations and give a clear physical interpretation.

Improved electromagnetic dissipation of Fe doping LaCoO_(3)toward broadband microwave absorption

Perovskite LaCoO_(3)is of great potential in electromagnetic wave absorption considering its outstanding dielectric loss as well as the existing magnetic response with the magnetic doping.However,the dissipation mechanism of the magnetic doping on the microwave absorption is lack of sufficient investigated.In this paper,LaCo_(1-x)Fe_(x)O_(3)(x=0,0.05,0.1,0.15,0.2,0.25,0.3,LCFOs)perovskites with different Fe doping amounts were prepared successfully by the sol-gel method and subsequent heat treatment in the air atmosphere.The structure characterization carried out by the frst-principles calculations shows the effect of Fe doping on the dielectric and magnetic properties of LCFOs and the strong hybridization of Co/Fe-3d with O-2p in the LCFOs system was successfully demonstrated.Particularly,when x=0.1 and the thickness is only 1.95 mm,the LaCo_(0.9)Fe_(0.1)O_(3)exhibits the best microwave absorption performance with the minimum reflection loss(RL)value of about-41 dB.The typical samples achieve a broad effective absorption bandwidth(EAB)of 5.16 GHz(7.92-13.08 GHz),which covers the total X band(8-12 GHz).Considering that,the especial Fe doping perovskite is promising to be a candidate as efficient microwave absorbers.

Reversible magnetism transition at ferroelectric oxide heterointerface

Oxide heterointerface is a platform to create unprecedented two-dimensional electron gas, superconductivity and ferromagnetism, arising from a polar discontinuity at the interface. In particular, the ability to tune these intriguing effects paves a way to elucidate their fundamental physics and to develop novel electronic/magnetic devices. In this work, we report for the first time that a ferroelectric polarization screening at SrTiO_(3)/PbTiO_(3) interface is able to drive an electronic construction of Ti atom, giving rise to room-temperature ferromagnetism. Surprisingly, such ferromagnetism can be switched to antiferromagnetism by applying a magnetic field, which is reversible. A coupling of itinerant electrons with local moments at interfacial Ti3d orbital was proposed to explain the magnetism. The localization of the itinerant electrons under a magnetic field is responsible for the suppression of magnetism. These findings provide new insights into interfacial magnetism and their control by magnetic field relevant interfacial electrons promising for device applications.

Stability and electronic structure studies of LaAlO_3/SrTiO_3 (110) heterostructures

The first-principles calculations are employed to investigate the stability, magnetic, and electrical properties of the oxide heterostructure of LaAIO3/SrTiO3 （110）. By comparing their interface energies, it is obtained that the buckled interface is more stable than the abrupt interface. This result is consistent with experimental observation. At the interface of LaAIO3/SrTiO3 （110） heterostructure, the Ti-O octahedron distortions cause the Ti tzg orbitals to split into the two- fold degenerate dxz/dyz and nondegenerate dxy orbitals. The former has higher energy than the latter. The partly filled two-fold degenerate t2g orbitals are the origin of two-dimensional electron gas, which is confined at the interface. Lattice mismatch between LaA103 and SrTiO3 leads to ferroelectric-like lattice distortions at the interface, and this is the origin of spin-splitting of Ti 3d electrons. Hence the magnetism appears at the interface of LaAIO3/SrTiO3 （110）.

Magnetic proximity effect induced spin splitting in two-dimensional antimonene/Fe_(3)GeTe_(2) van der Waals heterostructures

Recently, two-dimensional van der Waals(vd W) magnetic heterostructures have attracted intensive attention since they can show remarkable properties due to the magnetic proximity effect. In this work, the spin-polarized electronic structures of antimonene/Fe_(3)GeTe_(2)vdW heterostructures were investigated through the first-principles calculations. Owing to the magnetic proximity effect, the spin splitting appears at the conduction-band minimum(CBM) and the valence-band maximum(VBM) of the antimonene. A low-energy effective Hamiltonian was proposed to depict the spin splitting. It was found that the spin splitting can be modulated by means of applying an external electric field, changing interlayer distance or changing stacking configuration. The spin splitting energy at the CBM monotonously increases as the external electric field changes from-5 V/nm to 5 V/nm, while the spin splitting energy at the VBM almost remains the same. Meanwhile,as the interlayer distance increases, the spin splitting energies at the CBM and VBM both decrease. The different stacking configurations can also induce different spin splitting energies at the CBM and VBM. Our work demonstrates that the spin splitting of antimonene in this heterostructure is not singly dependent on the nearest Sb–Fe distance, which indicates that magnetic proximity effect in heterostructures may be modulated by multiple factors, such as hybridization of electronic states and the local electronic environment. The results enrich the fundamental understanding of the magnetic proximity effect in two-dimensional vdW heterostructures.

Atomic origin of magnetic coupling of antiphase boundaries in magnetite thin films

Revealing the magnetic coupling nature of boundary defects is crucial for in-depth understanding of the behavior and properties of magnetic materials and devices.Here,magnetite(i.e.,Fe_(3)O_(4))thin films were grown epitaxially on(100)SrTiOsingle-crystal substrates by pulsed laser deposition.Atomic-scale scanning transmission electron microscopy characterizations reveal that three types of antiphase boundaries(APBs)are formed in the Fe_(3)O_(4)thin film.They are the(100)APB that is formed on the(100)plane with a crystal translation of(1/4)a[011^(-)],the typeⅠand typeⅡ(110)APBs that are both formed on the(110)plane with the same crystal translation of(1/4)a[101]but different terminated atomic planes.The typeⅠ(110)APB is terminated at the atomic plane with mixed tetrahedral-and octahedral-sites Fe atoms,the typeⅡ(110)APB is terminated at the octahedral-site Fe plane.First-principles calculations reveal that the(100)APB and the typeⅠ(110)APB tend to form the ferromagnetic coupling that will not decrease the spin polarization of Fe_(3)O_(4)films,while the typeⅡ(110)APB prefers to form the antiferromagnetic coupling that will degrade the magnetic properties.The magnetic coupling modes of the APBs are closely related to the Fe-O-Fe bond angles across the boundaries.

Negative differential friction coefficients of two-dimensional commensurate contacts dominated by electronic phase transition

Friction force(f)usually increases with the normal load(N)macroscopically,according to the classic law of Da Vinci–Amontons(f=μN),with a positive and finite friction coefficient(μ).Herein near-zero and negative differential friction(ZNDF)coefficients are discovered in two-dimensional(2D)van der Waals(vdW)magnetic CrI_(3)commensurate contacts.It is identified that the ferromagnetic–antiferromagnetic phase transition of the interlayer couplings of the bilayer CrI_(3)can significantly reduce the interfacial sliding energy barriers and thus contribute to ZNDF.Moreover,phase transition between the in-plane(p_(x)and p_(y))and out-of-plane(p_(z))wave-functions dominates the sliding barrier evolutions,which is attributed to the delicate interplays among the interlayer vdW,electrostatic interactions,and the intralayer deformation of the CrI_(3)layers under external load.The present findings may motivate a new concept of slide-spintronics and are expected to play an instrumental role in design of novel magnetic solid lubricants applied in various spintronic nano-devices.