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La0.7Sr0.3MnO3, a strong semi-metallic ferromagnet having robust spin polarization and magnetic transition temperature (TC) well above 300 K, has attracted significant attention as a possible candidate for a wide range of memory, spintronic, and multifunctional devices. Since varying the oxygen partial pressure during growth is likely to change the structural and other physical functionalities of La0.7Sr0.3MnO3 (LSMO) films, here we report detailed investigations on structure, along with magnetic behavior of LSMO films with same thickness (~30 nm) but synthesized at various oxygen partial pressures: 10, 30, 50, 100, 150, 200 and 250 mTorr. The observation of only (00 l) reflections without any secondary peaks in the XRD patterns confirms the high-quality synthesis of the above-mentioned films. Surface morphology of the films reveals that these films are very smooth with low roughness, the thin films synthesized at 150 mTorr having the lowest average roughness. The increasing of magnetic TC and sharpness of the magnetic phase transitions with increasing oxygen growth pressure suggests that by decreasing the oxygen growth pressure leads to oxygen deficiencies in grown films which induce oxygen inhomogeneity. Thin films grown at 150 mTorr exhibits the highest magnetization with TC = 340 K as these thin films possess the lowest roughness and might exhibit lowest oxygen vacancies and defects. Interpretation and significance of these results in the 30 nm LSMO thin films prepared at different oxygen growth pressures are also presented, along with the existence and growth pressure dependence of negative remanent magnetization (NRM) of the above-mentioned thin films.

Aspects of the optoelectronic performance of thin-film ferromagnetic materials are evaluated for application in ultrafast devices. Dynamics of photocarriers and their associated spin polarization are measured using transient reflectivity (TR) measurements in cross linear and circular polarization configurations for La0.7Sr0.3MnO3 films with a range of thicknesses. Three spin-related recombination mechanisms have been observed for thicker films (thickness of d ≥ 20 nm) at different time regimes (τ), which are attributed to the electron–phonon recombination (τ 1 ns). Density functional theory (DFT+U) based first-principles calculations provide information about the nature of the optical transitions and their probabilities for the majority and the minority spin channels. These transitions are partly responsible for the aforementioned recombination mechanisms, identified through the compari...

CuAlO2 is among several ternary delafossites in which the electronic bandgap is less than the optical bandgap due to Laporte selection rules. Because alloying is expected to provide band engineering in delafossites, we are investigating Fe-doped CuAlO2. Here, results from the detailed magnetic characterization of the CuAl1−xFexO2 (x = 0.0, 0.01, 0.05, and 0.1) samples, prepared by a solid-state reaction of Cu2O, Al2O3, and Fe2O3, at 1100 °C, are reported. X-ray diffraction (XRD) of the powder samples showed an expansion of the rhombohedral unit cell with increasing x showing that the larger Fe3+ (r = 0.645 A) is replacing the smaller Al3+ion (r = 0.535 A). The analysis of magnetization (M) vs. temperature (T, from 2 to 300 K) data in terms of the Curie-Weiss law: M = CH/(T − θ) confirms Fe3+ as the electronic state of Fe with spin S = 5/2 (magnetic moment μ = 5.9 μB) as determined from the Curie constant, C; this analysis also yields a negative θ characteristic of an antiferromagnetic Fe3+–Fe3+ exchange coupling and magnitudes of x in good agreement with the nominal values. The isothermal M vs. H (up to H = 90 kOe) data analyzed in terms of modified Brillouin function involving H/(T − θ) support the results obtained from the M vs. T analysis. The small paramagnetism observed in undoped CuAlO2 is related to the presence of a few percent of CuAl2O4 impurity observed in XRD of the sample.

The properties of many materials can be strongly affected by the atomic valence of the contained individual elements, which may vary at surfaces and other interfaces. These variations can have a critical impact on material performance in applications. A non-destructive method for the determination of layer-by-layer atomic valence as a function of material thickness is presented for La0.7Sr0.3MnO3 (LSMO) thin films. The method utilizes a combination of bulk- and surface-sensitive X-ray absorption spectroscopy (XAS) detection modes; here, the modes are fluorescence yield and surface-sensitive total electron yield. The weighted-average Mn atomic valence as measured from the two modes are simultaneously fitted using a model for the layer-by-layer variation of valence based on theoretical model Hamiltonian calculations. Using this model, the Mn valence profile in LSMO thin film is extracted and the valence within each layer is determined to within an uncertainty of a few percent. The approach presented here could be used to study the layer-dependent valence in other systems or extended to different properties of materials such as magnetism.

Films of CuFeO2 and CuFe0.75Ga0.25O2 were grown over sapphire substrates in high vacuum using a pulsed laser deposition technique. The films grew with rhombohedral delafossite structure and highly epitaxial in the c-direction. Samples were characterized by X-ray diffraction, Raman spectroscopy and atomic force microscopy. Surface of the films were inspected with X-ray and UV photoelectron spectroscopy. Adsorption of CO2 and H2O was studied by a thermal program desorption technique. In both films Cu and Fe were exposed at the surface–gas interface. X-ray photoelectron data indicated that CO2 adsorbs preferentially at Cu sites forming a similar coordination to CuCO3. The energy for desorption of CO2 and H2O was estimated to be 30 kcal mol−1 (1.3 eV atom−1) for CuFeO2 and 36 kcal mol−1 (1.6 eV mol−1) for CuFe0.75Ga0.25O2. UV photoelectron spectroscopy showed that the valence band of the CuFeO2 delafossite oxides is modified with the substitution of Fe by Ga in the crystal lattice. The semiconductor band gap of CuFeO2 delafossite oxides also increased from 1.2 to 1.5 eV due to the substitution of Fe by Ga in the crystal lattice.

Transient reflectivity (TR) measurements for La0.7Sr0.3MnO3 thin films indicate enhanced surface recombination of charge carriers for thinner films (d < 20 nm). Wavelet analysis of residual TR shows abrupt oscillatory modes with close energy ranges.

We report a detailed investigation on magnetic and electrical properties of the multiferroic GaFeO3 (GFO) thin films grown on SrRuO3 (SRO) buffered SrTiO3 (1 1 1) substrates. The magnetic transition temperature (Tc) of GFO thin films is observed ∼240 K, which is higher by 20 K than in GFO ceramic. The clear and reversible out-of-plane phase-contrast seen in the Piezoresponse Force Microscopy (PFM) phase and amplitude images measured within positive and negative poling confirms the polarization reorientation and hence piezoelectric nature of the compound. The temperature and frequency dependence of permittivity studies demonstrates the relaxor behavior of these thin films. The observed near room temperature (RT) magnetic phase transition with RT piezoelectric nature of these thin films elucidates the possible potential candidates for a multiferroic world with spintronics device applications.

Analysis of the results from our investigations of the temperature dependence of ac susceptibilities ( χ ′ and χ ′ ′) and magnetic viscosity in a 7.6 nm thin film of La0.7Sr0.3MnO3 grown on SrTiO3 (001) substrate is presented. The Curie temperature (TC) of this film is magnetic field (H) dependent, varying as [ T C ( H ) − T C ( 0 ) ] ∼ H n with TC(0) = 270 K and n = 0.15. Temperature dependence of χ ′ and χ ′ ′ measured at ac frequencies fm in the range of 0.1–10 kHz shows a broad peak near 230 K associated with the blocking temperature ( T B ) of spin clusters present in the 1.4 nm surface layer and a frequency dependent peak near 270 K associated with T C. The mean relaxation time τ determined from the Cole–Cole analysis of the temperature dependent χ ′ and χ ′ ′ is shown to fit the Vogel–Fulcher law: τ = τ 0 exp [ Δ E / k B ( T − T 0 ) ] with T0 = 245 K, ΔE/kB = 270 K = TC, and τ0 = 1.2 × 10−9 s. Magnetic viscosity S (measured in H = 0 for a sample cooled in H = 50 Oe) determined from the fit to the magnetization: M (t) = M (0) – S ln t, with time t up to 2 h, shows a peak at 230 K above which M (2 h) switches to negative values for temperatures up to TC(0). It is argued that this negative magnetization results from an interaction between the superparamagnetic spin clusters and the ferromagnetic phase, both being present in the temperature range of TB

Modifying Fe and Mn contents in GaFeO3 (GFO) enhances the magnetic properties, increases the magnetic transition temperature (TC) and reduces the leakage current. Here, we report structural, magnetic, and leakage current characteristics of manganese-doped gallium ferrite with different Fe-content, i.e. Ga2−xFexO3 (1 ≤ x ≤ 1.4) system. Structural characterization reveals that all the samples retain the orthorhombic phase with space group Pc21n for above amounts of doping. Magnetization of the samples with respect to temperature shows the lower magnetic transition temperature (TC) for pure GFO, i.e. 220 K, which increases to 345 K above room temperature (RT) for 2% Mn-doped Ga0.6Fe1.4O3 (GFMO3). Higher remanent magnetization (~16 emu g−1) with a lower coercive field (~4 kOe) is obtained for Mn-doped Ga0.6Fe1.4O3. We found the decrease of leakage current with doping of Mn. The observation of multiferroicity in these single-phase materials (i.e. GFO3 and GFMO3) at RT make them potential candidates for memory, multifunctional, and spintronics device applications.

The Mn valence in thin film La0.7Sr0.3MnO3 was studied as a function of film thickness in the range of 1–16 unit cells with a combination of non-destructive bulk and surface sensitive X-ray absorption spectroscopy techniques. Using a layer-by-layer valence model, it was found that while the bulk averaged valence hovers around its expected value of 3.3, a significant deviation occurs within several unit cells of the surface and interface. These results were supported by first principles calculations. The surface valence increases to up to Mn3.7+, whereas the interface valence reduces down to Mn2.5+. The change in valence from the expected bulk value is consistent with charge redistribution due to the polar discontinuity at the film-substrate interface. The comparison with theory employed here illustrates how this layer-by-layer valence evolves with film thickness and allows for a deeper understanding of the microscopic mechanisms at play in this effect. These results offer insight on how the two-dimensional electron gas is created in thin film oxide alloys and how the magnetic ordering is reduced with dimensionality.

The depth-dependent magnetization in thin film oxygen stoichiometric and oxygen-deficient La0.7Sr0.3MnO3 is investigated by using polarized neutron reflectivity and DC bulk magnetometry. The polarized neutron reflectivity results reveal that the stoichiometric sample shows enhanced interfacial magnetization relative to the rest of the film. The oxygen-deficient sample exhibits a reduced average magnetization from the optimized recipe. Both films show regions of suppressed magnetization at the surface regardless of the growth pressure. The oxygen stoichiometric film does not show an interfacial dead layer, whereas the oxygen-deficient film exhibits a dead layer whose thickness changes with temperature. At a low applied field, we observe striking differences in the depth dependence of the magnetic ordering, with the oxygen-deficient film exhibiting exchange spring behavior, while the stoichiometric film shows a constant magnetization direction across the film. These results suggest that the incorporation of oxygen vacancies during growth leads to an accumulation of vacancies at the interface, which is enhanced at higher temperature due to increased oxygen mobility, creating a region of reduced magnetism that couples to the rest of the film. These results offer insight into the complex behavior and role of oxygen vacancies in the magnetism of these systems. Additionally, the study reveals further details of the negative magnetization in La0.7Sr0.3MnO3 reported in previous studies, which are discussed here.

Applications of wavelet analysis in ultra-thin film transient reflectivity (TR) measurements have been investigated. Advantages of utilizing different localized wavelet bases, in position and time, have been addressed on the residual TR signals. Morse wavelets have been used to obtain information from the abrupt oscillatory modes in the signal, which are not distinguishable with conventional methods such as Fourier transforms. These abrupt oscillatory modes are caused by the surface, interface, or any short-lived oscillatory modes which are suppressed in the TR signal in ultra-thin films. It is demonstrated that by choosing different Morse wavelets, information regarding different oscillatory modes in the TR signal of a heterostructure thin film is achievable. Moreover, by performing wavelet analysis on multiferroic heterostructures, oscillatory modes with very close energy ranges are easily distinguishable. For illustration, residuals of the TR signals have been obtained by a pump-probe setup in reflectivity mode on La0.7Sr0.3MnO3/SrTiO3 and BaTiO3/La0.7Sr0.3MnO3/SrTiO3 samples, where sufficient signal to noise ratios have been achieved by taking multiple scans. The residual signals have been analyzed with Morse wavelets, and multiple oscillatory modes with close energy ranges have been observed and distinguished. This approach can isolate the location of various oscillatory modes at the surface, interface and in the bulk of the heterostructure sample.

Low-energy collective electronic excitations exhibiting sound-like linear dispersion have been intensively studied both experimentally and theoretically for a long time. However, coherent acoustic plasmon modes appearing in time-domain measurements are rarely observed due to Landau damping by the single-particle continua. Here we report on the observation of coherent acoustic Dirac plasmon (CADP) modes excited in indirectly (electrostatically) opposite-surface coupled films of the topological insulator Bi2Se3. Using transient second-harmonic generation, a technique capable of independently monitoring the in-plane and out-of-plane electron dynamics in the films, the GHz-range oscillations were observed without corresponding oscillations in the transient reflectivity. These oscillations were assigned to the transverse magnetic and transverse electric guided CADP modes induced by the evanescent guided Lamb acoustic waves and remained Landau undamped due to fermion tunnelling between the opposite-surface Dirac states., Coherent acoustic plasmons in time-domain measurements are rarely observed due to Landau damping. Here, Glinka et al. use transient second-harmonic generation to observe coherent acoustic Dirac plasmon modes survived in indirectly opposite-surface coupled Bi2Se3 films due to Dirac fermion tunnelling.

© 2016 IOP Publishing Ltd. Transient reflectivity (TR) measured at laser photon energy 1.51 eV from the indirectly intersurface-coupled topological insulator Bi2-xMnxSe3films (12 nm thick) revealed a strong dependence of the rise-time and initial decay-time constants on photoexcited carrier density and Mn content. In undoped samples (x = 0), these time constants are exclusively governed by electron-electron and electron-phonon scattering, respectively, whereas in films with x = 0.013-0.27 ultrafast carrier dynamics are completely controlled by photoexcited electron trapping by ionized Mn2+acceptors and their dimers. The shortest decay-time (∼0.75 ps) measured for the film with x = 0.27 suggests a great potential of Mn-doped Bi2Se3films for applications in high-speed optoelectronic devices. Using Raman spectroscopy exploiting similar laser photon energy (1.58 eV), we demonstrate that due to indirect intersurface coupling in the films, the photoexcited electron trapping in the bulk enhances the electron-phonon interaction strength in Dirac surface states.

The observation of inverted magnetic hysteresis loops and negative magnetic remanence (NRM) in a 7.6 nm thin film of La0.7Sr0.3MnO3 grown on SrTiO3 substrates is reported. The film was grown employing pulsed laser deposition and characterized by reflection high-energy electron diffraction during growth and using x-ray reflectivity measurements post-growth. Magnetic properties of the film were measured from 5 K to 400 K under both the field-cooled (FC) and zero-field-cooled (ZFC) conditions. The observed results of inverted magnetic hysteresis loops and NRM are interpreted in terms of the co-existence of a magnetically inhomogeneous region consisting of superparamagnetic spin clusters with a blocking temperature T B = 240 K and the ferromagnetic state with an ordering temperature T C = 290 K. Hysteresis loop inversion is observed in the temperature region of T B

Experimental investigations of the magnetic dead layer in 7.6 nm thick film of La0.7Sr0.3MnO3 (LSMO) are reported. The dc magnetization (M) measurements for a sample cooled to T = 5 K in applied field H = 0 reveal the presence of negative remanent magnetization (NRM) in the M vs. H (magnetic field) measurements as well as in the M vs. T measurements in H = 50 Oe and 100 Oe. The M vs. T data in ZFC (zero-field-cooled) and FC (field-cooled) protocols are used to determine the blocking temperature TB in different H. Isothermal hysteresis loops at different T are used to determine the temperature dependence of saturation magnetization (MS), remanence (MR) and coercivity HC. The MS vs. T data are fit to the Bloch law, MS (T) = M0 (1 – BT 3/2), showing a good fit for T < 100 K and yielding the nearest-neighbor exchange constant J/kB ≅ 18 K. The variations of TB vs. H and HC vs. T are well described by the model often used for randomly oriented magnetic nanoparticles with magnetic domain diameter ≈ 9 nm present in the dead-layer of thickness d =1.4 nm. Finally, the data available from literature on the thickness (D) variation of Curie temperature (TC) and MS of LSMO films grown under 200, 150, and 0.38 mTorr pressures of O2 are analyzed in terms of the finite-size scaling, with MS vs. D data fit to MS (D) = MS(b)(1-d/D) yielding the dead layer thickness d = 1.1 nm, 1.4 nm and 2.4 nm respectively. Brief discussion on the significance of these results is presented.