Strain relaxation in the epitaxy of La2/3Sr1/3MnO3 grown by pulsed-laser deposition on SrTiO3(001)

With a Curie point at 370?K, the half-metal (La_0.7Sr_0.3)MnO₃ (LSMO) is one of the most interesting candidates for electronic devices based on tunnel magnetoresistance. SrTiO₃ (STO) is up to now the best substrate for the epitaxy of suitable thin films of LSMO. The pseudocubic unit cell of rhombohedral LSMO has a parameter a _LSMO such that (a _STO ? a _LSMO)/a _LSMO = +?0.83% (where a _STO is the parameter of cubic STO) and an angle of 90.26°. As strained growth is tetragonal, relaxation implies recovery of both the pseudocubic parameter and of the original angle. In the LSMO layers that we prepare by pulsed-laser deposition, we show that these two processes are quite independent. The angular distortion is partially recovered by twinning in films 25?nm thick, while recovery of the parameter never occurs in the thickness range that we explored (up to 432?nm). A relaxation, however, takes place above a thickness of 100?nm, associated with a transition from two-dimensional to three-dimensional columnar growth. It is accompanied by chemical fluctuations. Our magnetic measurements exhibit Curie temperatures and magnetic moments very close to the bulk values in those layers where the crystal parameter is strained but the angle partially relaxed.     

La1－xSrxMnO3/TiO2 (x=0.2, 0.15, 0.04)异质pn结的整流特性

采用磁控溅射法制备的La_1-xSr_xMnO₃ (LSMO)/TiO₂异质pn结表现出很好的整流特性.室温电流电压特性曲线显示随着Sr掺杂的增加，扩散电压增大，这可能由于Sr掺杂的增加导致载流子浓度增大所致.电流电压变温特性曲线显示随着测量温度的降低，扩散电压增大，这可能由于随着测量温度的变化导致界面电子结构的变化所致.值得提出的，异质pn结电阻随温度变化曲线表现出单层LSMO的金属绝缘相变特性，并且在低测量温度时表现出随着测量温度的降低结电阻增大，这可能是由于宽带隙的TiO₂的引入导致. 关键词： 异质结 整流特性 庞磁阻     

Properties of thin manganite films grown on semiconducting substrates for spintronics applications

La_0.7Sr_0.3MnO₃ (LSMO) manganite thin films were grown by pulsed plasma deposition on silicon (Si) and gallium arsenide (GaAs) substrates covered by an amorphous oxide. Manganite films are characterized by polycrystalline structure. Ferromagnetic transition is above room temperature and for 50 nm thick film the Curie temperature was as high as 325 K and 305 K for LSMO/SiO_x/Si and LSMO/AlO_x/GaAs, respectively.     

Finite size effect and phase diagram of ultra-thin La0.7Sr0.3MnO3

La_0.7Sr_0.3MnO₃ (LSMO) ultra-thin films have been grown by pulsed laser deposition in conditions optimized for cation stoichiometry and bulk-like physical properties in the thick limit. Through electrical transport and magnetic measurements, a phase diagram is constructed as a function of film thickness. With decreasing thickness, the LSMO films cross over at high temperatures from a paramagnetic metal to a paramagnetic insulator, and at low temperatures from a ferromagnetic metal to a ferromagnetic insulator, in close similarity to that observed for varying the electronic bandwidth in bulk manganites.     

Direct angle resolved photoemission spectroscopy and superconductivity of strained high-T c films

Since 1997 we systematically perform direct angle resolved photoemission spectroscopy (ARPES) on in-situ grown thin (<30 nm) cuprate films. Specifically, we probe low-energy electronic structure and properties of high-T _c superconductors (HTSC) under different degrees of epitaxial (compressive vs. tensile) strain. In overdoped and underdoped in-plane compressed (the strain is induced by the choice of substrate) ≈15 nm thin La_{2 − x} Sr _x CuO₄ (LSCO) films we almost double T _c to 40 K, from 20 K and 24 K, respectively. Yet the Fermi surface (FS) remains essentially two-dimensional. In contrast, ARPES data under tensile strain exhibit the dispersion that is three-dimensional, yet T _c drastically decreases. It seems that the in-plane compressive strain tends to push the apical oxygen far away from the CuO₂ plane, enhances the two-dimensional character of the dispersion and increases T _c, while the tensile strain acts in the opposite direction and the resulting dispersion is three-dimensional. We have established the shape of the FS for both cases, and all our data are consistent with other ongoing studies, like EXAFS. As the actual lattice of cuprates is like a ‘Napoleon-cake’, i.e. rigid CuO₂ planes alternating with softer ‘reservoir’, that distort differently under strain, our data rule out all oversimplified two-dimensional (rigid lattice) mean field models. The work is still in progress on optimized La-doped Bi-2201 films with enhanced T _c.      

The influence of surface roughness in X-ray resonant magnetic reflectivity experiments

We present simulations of X-ray resonant magnetic reflectivity (XRMR) spectra of the surface magnetic dead layer in La_1−x Sr _x MnO₃ (LSMO) films that take in account the effect of different forms of roughness that can be encountered experimentally. The results demonstrate a method to distinguish between surface (morphological) roughness, and two generic kinds of magnetic roughness at the buried interface between the surface dead layer and the fully magnetic bulk part of the film. We show that the XRMR technique can distinguish between different types of magnetic roughness at the dead layer/bulk interface only if the sample surface is nearly atomically flat (the morphological roughness is one unit cell or less). Furthermore, to distinguish between the two types of magnetic roughness, the simulations show that fitting of XRMR spectra out to very high incidence angles must be performed. In the specific case of LSMO films with a dead layer with average thickness of 4 unit cells, this corresponds to an incidence angle > 50^∘.     

The Sr content influence on the positive magnetoresistance in La1-xSrxMnO3/Si heterojunctions

<正>We fabricated La_(1-x)Sr_xMnO_3/Si(LSMO/Si) heterojunctions with different Sr doping concentrations(x = 0.1, 0.2,0.3) in LSMO and studied the Sr content influence on magnetoresistance(MR) ratio.The hetero junctions show positive MR and high sensitivity of MR ratio in a low applied magnetic field.The MR ratio is dependent on Sr content and the low Sr doping in LSMO causes a large positive MR in LSMO/Si junctions.The MR ratio for 0.1 Sr doping in the LSMO/Si heterostructure is 116%in 100 Oe(1 Oe=79.5775 A/m) at 210 K.The mechanism for the positive MR dependence on the doping density is considered to be the competition between the tunneling rate of electrons in e_g~1↑to t_(2g)↓band and that to e_g~2↑band at the interface region of LSMO.The experimental results are in agreement with those observed in La_(0.9)Sr_(0.1)MnO_3/SrNb_(0.01)Ti_(0.99)O_3 p-n junction.The results indicate that choosing low doping concentration to improve the low field sensitivity of the heterojunction devices is a very efficacious method.     

外延生长La0.7Sr0.3MnO3薄膜厚度对缺陷影响的慢正电子分析

采用脉冲激光沉积方法在(LaAlO₃)_0:3(Sr₂AlTaO₆)_0:7衬底上外延生长了La_0.7Sr_0.3MnO₃薄膜,并采用慢正电子束方法分析了薄膜在不同厚度和不同退火气氛下参数S的变化. 分析表明,薄膜中包含两种机制引入的氧空位,分别是薄膜生长气氛中氧压偏低造成薄膜的氧缺乏和由于薄膜应变引入空位型缺陷. 当薄膜厚度较薄时,应变造成的晶格畸变化比较大,当薄膜的厚度大于11 nm时,薄膜的应变驰豫已经比较完全. 原位退火的样品中正电子主要是被氧缺乏引起的氧空位捕获. 在氧气中退火的样品,S随厚度的变化反映了应变对薄膜微结构的影响.     

Modelling of structural domains and elastic strain calculation in rhombohedral La1−x Sr x MnO3 films on (110) SrTiO3

As reported in the literature, structural domains in (110) oriented rhombohedral La_{1? x} Sr _x MnO₃ (LSMO) films on (110) SrTiO₃ show a pattern with alternating domain widths and inclined domain walls. An appropriate one-dimensional periodic domain model was developed and the non-uniform strain field in a coherently grown film was calculated by applying the coherency-defect approach. The strain is sharply peaked at the junction of the domain walls and the film/substrate interface. The dependence of the equilibrium domain-width ratio and domain-pattern period on film thickness was determined by minimizing the sum of elastic and domain-wall energies. The proposed domain structure can be formed only in a certain range of the film's crystal-structure data compared to the substrate. Corresponding composition-dependent structure data of LSMO are compiled.     

Modulation of ultrafast laser-induced magnetization precession in BiFeO<Subscript>3</Subscript>-coated La<Subscript>0.67</Subscript>Sr<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript> thin films

The ultrafast laser-excited magnetization dynamics of ferromagnetic (FM) La_0.67Sr_0.33MnO₃ (LSMO) thin films with BiFeO₃ (BFO) coating layers grown by laser molecular beam epitaxy are investigated using the optical pump-probe technique. Uniform magnetization precessions are observed in the films under an applied external magnetic field by measuring the time-resolved magneto-optical Kerr effect. The magnetization precession frequencies of the LSMO thin films with the BFO coating layers are lower than those of uncoated LSMO films, which is attributed to the suppression of the anisotropy field induced by the exchange interaction at the interface between the antiferromagnetic order of BFO and the FM order of LSMO.     

Electronic states near fermi level in superconductors La2 − x Sr x CuO4 by means of x-ray absorption spectra near Cu-K and La-L edges

The electronic states of La_{2? x} Sr _x CuO₄ with 0.00 ≤ x ≤ 0.20 are studied by means of X-ray absorption spectroscopy (XANES, EXAFS) near the K-edge of Cu²⁺ ion and the L-edges of La³⁺ ion. It is found that characteristic white lines occurring near L _II and L _III edges of La³⁺ ion show a slight energy shift depending on substituted Sr²⁺ ions, x and temperature. The white lines suggest that unoccupied high-density 5dπ and 5dδ bands of La³⁺ ion just above a Fermi level transform to a hybridized single band of 5dπδ at 78?K in the superconductors with x = 0.10, 0.16 and 0.20. On the other hand, the XANES spectra near the Cu-K edge including a pre-edge region do not depend on x and temperature in the region of 0.00 ≤ x ≤ 0.20. It is considered that there is no reconstruction of electronic states at the Fermi level in a Mott–Hubbard band gap between an O 2p valence band and a Cu 3d conduction band. The electronic states at the Fermi level are probably consisted of the unoccupied 5dπδ band and an empty charge-transfer 3d?⁹ L band at low temperature, bands of which occur in a band gap between a filled O 2p valence band and an unoccupied O 2p conduction band. The insulator–superconductor–metal transitions in La_{2? x} Sr _x CuO₄ are related to the 5dπδ and 3d?⁹ L bands and holes, which site at a top region of the O 2p valence band near the Fermi level produced by a substitution of La³⁺ with Sr²⁺ ions.     

Capacitance of the La0.67Sr0.33MnO3/(Ba,Sr)TiO3 interface induced by electric field penetration into the manganite electrode

(001)La_0.67Sr_0.33MnO₃/(001)(Ba_xSr_{1 ? x} TiO₃/(001)La_0.67Sr_0.33MnO₃(x= 0–0.25) three-layer heterostructures are grown by laser evaporation on (001)La_0.3Sr_0.7Al_0.65Ta_0.35O₃ single-crystalline substrates. In a wide temperature range (≈150 K), effective permittivity ? of (1000 nm)Ba_0.25Sr_0.75TiO₃ and (1000 nm)SrTiO₃ films grown obeys the relationship ? ～ (T ? T _CW)^?1, where T _CW is the Curie-Weiss temperature for related bulk crystals. Using experimental dependences ?(T), the capacitance of the (001)La_0.67Sr_0.33MnO₃/(001)Ba_xSr_1?x TiO₃ and (001)La_0.67Sr_0.33MnO₃/(001)SrTiO₃ interfaces, which is due to electric field penetration into the manganite electrode, is estimated (C _int≈4μF/cm²). At bias voltages of ± 2.5 V, the change in the permittivity of the STO and BSTO films in the heterostructures studied reaches 25 and 45%, respectively.     

Influence of microstructures on exchange bias behaviors of La0.7Sr0.3MnO3/La0.33Ca0.67MnO3 bilayers

Ferromagnetic La_0.7Sr_0.3MnO₃ (LSMO) and antiferromagnetic La_0.33Ca_0.67MnO₃ (LCMO) layers were grown on SrTiO₃ (STO) substrates by the pulsed laser deposition technique. LSMO films had rougher surfaces and larger grain sizes than LCMO films. Fully strained bilayers, in which each layer was as thin as 10 nm, were prepared by changing their stacking sequences, i.e. LSMO/LCMO/STO and LCMO/LSMO/STO. The former had higher T_C (350 K) than the latter (300 K), and exchange bias effects were only observed in the former bilayers. This revealed that microstructures could play an important role in the transport and magnetic properties of manganese oxide thin films.     

Magnetotransport characteristics of strained La<Subscript>0.7</Subscript>Sr<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> epitaxial manganite films

The electrical and magnetic characteristics of La_0.7Sr_0.3MnO₃ (LSMO) epitaxial manganite films are investigated by different methods under conditions when the crystal structure is strongly strained as a result of mismatch between the lattice parameters of the LSMO crystal and the substrate. Substrates with lattice parameters larger and smaller than the nominal lattice parameter of the LSMO crystal are used in experiments. It is shown that the behavior of the temperature dependence of the electrical resistance for the films in the low-temperature range does not depend on the strain of the film and agrees well with the results obtained from the calculations with allowance made for the interaction of electrons with magnetic excitations in the framework of the double-exchange model for systems with strongly correlated electronic states. Investigations of the magneto- optical Kerr effect have revealed that an insignificant (0.3%) orthorhombic distortion of the cubic lattice in the plane of the NdGaO₃(110) substrate leads to uniaxial anisotropy of the magnetization of the film, with the easy-magnetization axis lying in the substrate plane. However, LSMO films on substrates (((LaAlO₃)_0.3+(Sr₂AlTaO₆)_0.7)(001)) ensuring minimum strain of the films exhibit a biaxial anisotropy typical of cubic crystals. The study of the ferromagnetic resonance lines at a frequency of 9.76 GHz confirms the results of magnetooptical investigations and indicates that the ferromagnetic phase in the LSMO films is weakly inhomogeneous.     

Effect of Au proximity on the LSMO surface: An ab initio study

The effect of the proximity of Au on the electronic and magnetic properties of La_0.66Sr_0.33MnO₃ (LSMO) has been investigated by means of ab initio calculations within the density-functional theory. The calculations show an orbital reconstruction of the interfacial Mn, which is due more to the presence of a discontinuity rather than to a real chemical interaction with Au atoms. In fact, the same orbital reconstruction is found in the free LSMO surface. In both cases of Au/LSMO and LSMO surface, the Mn magnetic moments change very little with respect to the bulk case. In general, the calculations show a negligible influence of the Au atomic layer on LSMO at an ideal interface, with the LSMO surface magnetic and electronic properties essentially unchanged.     

Structure and magnetic properties of CrN thin films on La0.67Sr0.33MnO3

High crystalline quality CrN thin films have been grown on La_0.67Sr_0.33MnO₃ (LSMO) templates by molecular beam epitaxy. The structure and magnetic properties of CrN/LSMO heterojunctions are investigated combining with the experiments and the first-principles simulation. The Nėel temperature of the CrN/LSMO samples is found to be 281 K and the saturation magnetization of CrN/LSMO increases compared to that of LSMO templates. The magnetic property of CrN/LSMO heterostructures mainly comes from Cr atoms of (001) CrN and Mn atoms of (001) LSMO. The (001) LSMO induces and couples the spin of the CrN sublattice at CrN/LSMO interface.     

Microstructures and electrical properties of La0.8Sr0.2MnO3 films synthesized by sol-gel method

La_0.8Sr_0.2MnO₃ (LSMO) thin films were fabricated on alumina substrates by an improved sol-gel dip-coating process. It was found that multiple dip-coating process could not be performed until the pre-firing temperature reached 600 °C. Different amounts of LSMO powders were added to precursor solution with an aim to avoid cracks in LSMO thin films during calcining caused by the shrinkage mismatch between the film and the substrate. The structure and surface morphology of the films prepared from precursors with and without LSMO powders were characterized using X-ray diffraction (XRD) and scanning electron microscopy (SEM). It was found that the addition of 56.4 wt.% LSMO powders into the sol-gel precursor solution significantly modified the microstructure of films. A single LSMO perovskite phase was obtained on alumina substrate after calcining at 800 °C for 4 h by the improved sol-gel method. The sheet resistance of the films prepared with different processing parameters was measured by four-point dc method. Results indicated that the sheet resistance of films decreased with increasing the number of coating applications and the amount of LSMO powders.     

Growth mechanism, microstructure and transport properties of Sr1−x La x CuO2 (x=0.10−0.15) thin films

Sr_1−x La _x CuO₂ (x=0.10−0.15) thin films with an infinite-layer type structure were grown on BaTiO₃ buffered (001) SrTiO₃ substrates by pulsed laser deposition (PLD). The evolution of the growth front was monitored, in-situ, by high-pressure reflection high-energy electron diffraction (RHEED), while the surface morphology was analyzed by means of atomic force microscopy (AFM), ex-situ. X-ray diffraction (XRD) was used to determine the evolution of the film structure with deposition and cooling parameters, as well as to study the type and level of epitaxial strain in the Sr_1−x La _x CuO₂ films. The RHEED data showed that the Sr_1−x La _x CuO₂ films grow on BaTiO₃/SrTiO₃ following a 2D or Stranski-Krastanov mechanism, depending on the La doping level. The transition point (critical thickness d _c) from layer-by-layer like (2D) to island (3D) growth depends on the film stoichiometry: decreasing the La doping concentration x from 0.15 to 0.10, the critical thickness d _c increases from ∼45 nm to ∼75 nm. In order to induce superconductivity, the Sr_1−x La _x CuO₂ films were cooled down under reduction conditions. The as-deposited films showed semiconducting or metallic behavior, the resistivity decreasing with increasing La concentration. Post-deposition vacuum annealing resulted in a superconducting transition onset (but no zero resistance down to 4.2 K) only for some of the x=0.15 Sr_1−x La _x CuO₂ films.     

Laser-induced voltage (LIV) enhancement of La2/3Sr1/3MnO3 films with Ag addition

La_2/3Sr_1/3MnO₃:Ag _x (LSMO:Ag _x , x=0, 0.04, 0.08, 0.10, 0.20, 0.30) films were grown on vicinal cut LaAlO₃ (LAO) substrates by pulsed laser deposition technique (PLD). It is found that laser-induced voltage (LIV) of LSMO:Ag _x films is improved and enhanced by Ag addition. With x increasing, figure of merit (F _m ) and anisotropic Seebeck coefficient (ΔS) of LSMO:Ag _x (x=0.08) films reach the maximum values of 28.25 mV/ns and 0.38 μV/K, respectively. The results suggest that the LIV enhancement of LSMO:Ag _x films is due to the anisotropy of the Seebeck tensor, which is produced by long range cooperative Jahn–Teller distortions with Ag addition.     

Influence of oxygen reduction on the structural and electronic properties of electron-doped Sr1−xLaxCuO2 thin films

Single-phase, c-axis oriented, e-doped, Sr_1?xLa_xCuO₂ thin films were epitaxially grown on KTaO₃ and DyScO₃ substrates by reactive rf sputtering. As-grown films being insulating due to oxygen excess, oxygen reduction is necessary to observe superconductivity. Two different procedures were employed to reach superconductivity. On one hand an in situ reduction process was conducted on a series of films deposited on both type of substrates. On the other hand, an ex situ reduction procedure was performed sequentially on a single film deposited on DyScO₃. The study of the influence of oxygen reduction on the structural and electronic properties of the thin films is presented and discussed.