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Coordinate descent methods have considerable impact in global optimization because global (or, at least, almost global) minimization is affordable for low-dimensional problems. Coordinate descent methods with high-order regularized models for smooth nonconvex box-constrained minimization are introduced in this work. High-order stationarity asymptotic convergence and first-order stationarity worst-case evaluation complexity bounds are established. The computer work that is necessary for obtaining first-order $\varepsilon$-stationarity with respect to the variables of each coordinate-descent block is $O(\varepsilon^{-(p+1)/p})$ whereas the computer work for getting first-order $\varepsilon$-stationarity with respect to all the variables simultaneously is $O(\varepsilon^{-(p+1)})$. Numerical examples involving multidimensional scaling problems are presented. The numerical performance of the methods is enhanced by means of coordinate-descent strategies for choosing initial points.

The sensitivity and automation capabilities of modern superconducting quantum interference device (SQUID) magnetometers are currently unmatched. The measured moment values are, however, prone to deviations from their actual value due to geometric effects, namely sample size, shape, and radial offset. This is well known, and a knowledgeable operator will correct measured moment values taking these effects into account. The current procedure for the Magnetic Property Measurement 3 (MPMS3) magnetometer is based on an available simulation tool, valid for both Vibrating Sample Magnetometer (VSM) and Direct Current (DC) methods. Still, determining the correction factor requires samples with well-defined geometric shapes together with accurate sample dimensions and the usually difficult to determine radial offset. Additionally, at the moment, there is not a proper solution to correct geometry effects of irregular shaped samples. In this work, we find a systematic relation between the difference between the VSM and DC measurements and their corresponding correction factors for MPMS3 SQUID-VSM device. This relation follows a clear trend, independent of sample size, shape or radial offset, for a given pair of DC scan length and VSM amplitude values. Exploiting this trend, a geometry-independent correction method is here presented and validated by measurements of metallic Fe powder using a far from optimal sample mounting.

Heusler alloys are promising for several applications, including magnetic refrigeration, due to high magnetocaloric and magnetovolume effects. One way to optimize this potential is by increasing the magnetovolume effect. Using density functional theory with the Korringa-Kohn-Rostoker method, we calculate the effective exchange interaction energies and corresponding mean field Curie temperature as a function of the volume (hydrostatic pressure) in several L2 1 -type Co 2 YZ Heusler alloys. Different qualitative trends and signs of the pressure derivatives of the Curie temperature and moments are found among these compounds, discussed and compared with previous calculations and experiments., Comment: INTERMAG 2014 - IEEE International Magnetics Conference, Dresden, May 5-8, 2014. 3 pages, 5 figures

We report perturbed angular correlation measurements with 111mCd/111Cd and 111In/111Cd probes, at the ISOLDE-CERN facility, in the manganite compounds BaMnO3 , with the 6H and 15R polymorphs, and SrMnO3 , with the 4H polymorph. The electric field gradient (EFG) is measured, and found approximately constant in a large temperature range for all the compounds. The EFG is also calculated from first principles with density functional theory, and compared with experimental results by considering diluted substitutional Cd impurities. Based on the results, we assign as sites for the probes the Ba (for BaMnO3-6H, 15R) and Sr (for SrMnO3-4H) sites, apart from fractions of undetermined origin in the case of BaMnO3-6H. We predict the hyperfine parameters in the recently synthesized multiferroic manganite Sr0.5Ba0.5MnO3 , and its variation with the structure and electric polarization, which is found to be very small., Comment: 13 pages, 9 figures

The magnetic properties tuning and volume dependence in the series of quaternary full Heusler alloys with formula Co2Cr1-xYGa (Y = Ti, V, Mn, Fe, Co, Ni) were studied with a detailed first-principles exploration. We employ the density functional KKR method with the coherent potential approximation, estimating effective Heisenberg exchange constants via the magnetic force theorem together with mean-field Curie temperature (TC) and magnetic moment for compositions in the whole concentration range. The volumetric dependency of these magnetic properties is studied, particularly the pressure derivatives of TC at equilibrium. Our ternary alloy calculations show good agreement with local-density and generalized gradient approximations in the literature. The quaternary alloys show a wide range of tunable magnetic properties, where magnetic moments range from 0.8 to 4.9 mu_B, TC from 130 K to 1250 K, and dTC/dV values range from -7 to +6.3 K A-3.

Epitaxial La0.7Sr0.3MnO3 (LSMO) thin films, with different thickness ranging from 20 nm up to 330 nm, were deposited on (100)-oriented strontium titanate (STO) substrates by pulsed laser deposition, and their structure and morphology characterized at room temperature. Magnetic and electric transport properties of the as-processed thin films reveal an abnormal behavior in the temperature dependent magnetization M(T) below the antiferrodistortive STO phase transition (TSTO) and also an anomaly in the magnetoresistance and electrical resistivity close to the same temperature. Up to 100 nm LSMO thin films, an in-excess magnetization and pronounced changes in the coercivity are evidenced, achieved through the interface-mediated magnetoelastic coupling with antiferrodistortive domain wall movement occurring below TSTO. Contrarily, for thicker LSMO thin films, above 100 nm, an in-defect magnetization is observed. This reversed behavior can be understood within the emergence in the upper layer of the film, observed by high resolution transmission electron microscopy, of a branched structure needed to relax elastic energy stored in the film which leads to randomly oriented magnetic domain reconstructions. For enough high-applied magnetic fields, as thermodynamic equilibrium is reached, a fully suppression of the anomalous magnetization occurs, wherein the temperature dependence of the magnetization starts to follow the expected Brillouin behavior., Comment: 15 pages, 9 figures

The MnAs compound shows a first-order transition at T$_C\approx42$ C, and a second-order transition at T$_t\approx120$ C. The first-order transition, with structural (hexagonal-orthorhombic), magnetic (FM-PM) and electrical conductivity changes, is associated to magnetocaloric, magnetoelastic, and magnetoresistance effects. We report a study in a large temperature range from $-196$ up to $140$ C, using the $\gamma-\gamma$ perturbed angular correlations method with the radioactive probe $^{77}$Br$\rightarrow^{77}$Se, produced at the ISOLDE-CERN facility. The electric field gradients and magnetic hyperfine fields are determined across the first- and second-order phase transitions encompassing the pure and mixed phase regimes in cooling and heating cycles. The temperature irreversibility of the 1st order phase transition is seen locally, at the nanoscopic scale sensitivity of the hyperfine field, by its hysteresis, detailing and complementing information obtained with macroscopic measurements (magnetization and X-ray powder diffraction). To interpret the results, hyperfine parameters were obtained with first-principles spin-polarized density functional calculations using the generalized gradient approximation with the full potential (L)APW+lo method (\textsc{Wien2k} code) by considering the Se probe at both Mn and As sites. A clear assignment of the probe location at the As site is made and complemented with the calculated densities of states and local magnetic moments. We model electronic and magnetic properties of the chemically similar MnSb and MnBi compounds, complementing previous calculations., Comment: 21 pages, 11 figures

30 keV 111mCd and 50 keV 199mHg beams from ISOLDE were used to implant on preformed target of C60 with the thickness of 1 mg/cm2. Endofullerene compounds, viz.,111mCd@C60 and 199mHg@C60 formed during implantation were separated by filtration through micropore filter paper followed by solvent extraction. Dried samples of the endofullerene compounds were counted for the coincidence for the 151-245 keV cascade of 111mCd and 374-158 keV cascade for 199mHg for the TDPAC measurement on a six LaBr3 detector system coupled with digital electronics. The results indicate a single site occupied by the Cd atom in the fullerene cage with fast relaxation component which means that the Cd atom does move inside the cage at room temperature. The quadrupole interaction frequency and asymmetry parameter of the Cd atom occupying the site in C60 are WQ=8.14(42) Mrad/s and eta= 0.42(9) respectively with a site population of 28%. Fast relaxation constant is 0.003 ns-1 with a site contribution of 72%. On the other hand, Hg atom has two static sites of quadrupole frequencies, WQ1=281.60(16.9) Mrad/s and WQ2=202.30(22.7) Mrad/s. Respective asymmetry parameters are eta1=0.1(1) and eta2=0.2(1). The static components have a contribution of 40% with the rest 60% coming from the fast relaxing component., Comment: 12 pages, 4 figures one table

The charge ordered La$_{1/3}$Sr$_{2/3}$FeO$_{3-\delta}$ (LSFO) in bulk and nanocrystalline forms are investigated using ac and dc magnetization, M\"{o}ssbauer, and polarised neutron studies. A complex scenario of short range charge and magnetic ordering is realized from the polarised neutron studies in nanocrystalline specimen. This short range ordering does not involve any change in spin state and modification in the charge disproportion between Fe$^{3+}$ and Fe$^{5+}$ compared to bulk counterpart as evident in the M\"{o}ssbauer results. The refinement of magnetic diffraction peaks provides magnetic moments of Fe$^{3+}$ and Fe$^{5+}$ are about 3.15$\mu_B$ and 1.57$\mu_B$ for bulk, and 2.7$\mu_B$ and 0.53$\mu_B$ for nanocrystalline specimen, respectively. The destabilization of charge ordering leads to magnetic phase separation, giving rise to the robust exchange bias (EB) effect. Strikingly, EB field at 5 K attains a value as high as 4.4 kOe for average size $\sim$ 70 nm, which is zero for the bulk counterpart. A strong frequency dependence of ac susceptibility reveals cluster-glass like transition around $\sim$ 65 K, below which EB appears. Overall results propose that finite size effect directs the complex glassy magnetic behavior driven by unconventional short range charge and magnetic ordering, and magnetic phase separation appears in nanocrystalline LSFO., Comment: 10 pages, 9 figures. Fig. 1 available upon request or in http://www.ffn.ub.es/oscar/Articles.html. Accepted in Phys. Rev. B

The hyperfine interaction between the quadrupole moment of atomic nuclei and the electric field gradient (EFG) provides information on the electronic charge distribution close to a given atomic site. In ferroelectric materials, the loss of inversion symmetry of the electronic charge distribution is necessary for the appearance of the electric polarization. We present first-principles density functional theory calculations of ferroelectrics such as BaTiO3, KNbO3, PbTiO3 and other oxides with perovskite structures, by focusing on both EFG tensors and polarization. We analyze the EFG tensor properties such as orientation and correlation between components and their link with electric polarization. This work supports previous studies of ferroelectric materials where a relation between EFG tensors and polarization was observed, which may be exploited to study ferroelectric order when standard techniques to measure polarization are not easily applied., Comment: 9 pages, 6 figures, 5 tables, corrected typos, as published in Phys. Rev. B

We show that the coercive field in ferritin and ferrihydrite depends on the maximum magnetic field in a hysteresis loop and that coercivity and loop shifts depend both on the maximum and cooling fields. In the case of ferritin we show that the time dependence of the magnetization also depends on the maximum and previous cooling fields. This behavior is associated to changes in the intra-particle energy barriers imprinted by these fields. Accordingly, the dependence of the coercive and loop shift fields with the maximum field in ferritin and ferrihydrite can be described within the frame of a uniform-rotation model considering a dependence of the energy barrier with the maximum and the cooling fields., Comment: 8 pages, 5 figures. Accepted for publication in Phys. Rev. B. Final version with improved writing and figures

We show that antiferromagnetic susceptibility in ferritin increases with temperature between 4.2 K and 180 K (i. e. below the N\'{e}el temperature) when taken as the derivative of the magnetization at high fields ($30\times10^4$ Oe). This behavior contrasts with the decrease in temperature previously found, where the susceptibility was determined at lower fields ($5\times10^4$ Oe). At high fields (up to $50 \times10^4$ Oe) the temperature dependence of the antiferromagnetic susceptibility in ferritin nanoparticles approaches the normal behavior of bulk antiferromagnets and nanoparticles considering superantiferromagnetism, this latter leading to a better agreement at high field and low temperature. The contrast with the previous results is due to the insufficient field range used ($< 5 \times10^4$ Oe), not enough to saturate the ferritin uncompensated moment., Comment: 7 pages, 7 figures, accepted in Phys. Rev. B

A detailed study of the electric field gradient (EFG) across the Pr1-xCaxMnO3 phase diagram and its temperature dependence is given. Clearly, distinct EFG behaviours for samples outside/inside the charge order (CO) region are observed. The EFG temperature dependence evidences a new phase transition occurring over the broad CO region of the phase diagram. This transition is discontinuous and occurs at temperatures between the charge ordering and the Neel temperatures. The features observed in the EFG are associated with polar atomic vibrations which eventually lead to a spontaneous local electric polarization below CO transition., Comment: 8 pages, 4 figures

We show that the magnetic anisotropy energy of antiferromagnetic ferrihydrite depends on the square root of the nanoparticles volume, using a method based on the analysis of statistical distributions. The size distribution was obtained by transmission electron microscopy, and the anisotropy energy distributions were obtained from ac magnetic susceptibility and magnetic relaxation. The square root dependence corresponds to random local anisotropy, whose average is given by its variance, and can be understood in terms of the recently proposed single phase homogeneous structure of ferrihydrite., Comment: 6 pages, 2 figures

In this paper we present a thorough analysis of two systems magnetically inhomogeneous: the manganite La$_{0.7}$Sr$_{0.3}$MnO$_3$/MgO and the amorphous alloy Cu$_{90}$Co$_{10}$. In both cases, the non-extensive statistics yield a faithful description of the magnetic behavior of the systems. In the model proposed here, the inhomogeneous magnetic system is composed by many Maxwell-Boltzmann homogeneous bits and the entropic parameter $q$ is related to the moments of the distribution of the inhomogeneous quantity. From the analysis of Scanning Tunnelling Spectroscopy (STS) images, the $q$ parameter can be directly measured.

We show how to extract the $q$ parameter from experimental data, considering an inhomogeneous magnetic system composed by many Maxwell-Boltzmann homogeneous parts, which after integration over the whole system recover the Tsallis non-extensivity. Analyzing the cluster distribution of La$_{0.7}$Sr$_{0.3}$MnO$_{3}$ manganite, obtained through scanning tunnelling spectroscopy, we measure the $q$ parameter and predict the bulk magnetization with good accuracy. The connection between the Griffiths phase and non-extensivity is also considered. We conclude that the entropic parameter embodies information about the dynamics, the key role to describe complex systems., Comment: Submitted to Phys. Rev. Lett

In this work, we report an atomic scale study on the ferromagnetic insulator manganite LaMnO$_{3.12}$ using $\gamma-\gamma$ PAC spectroscopy. Data analysis reveals a nanoscopic transition from an undistorted to a Jahn-Teller-distorted local environment upon cooling. The percolation thresholds of the two local environments enclose a macroscopic structural transition (Rhombohedric-Orthorhombic). Two distinct regimes of JT-distortions were found: a high temperature regime where uncorrelated polaron clusters with severe distortions of the Mn$^{3+}$O$_{6}$ octahedra survive up to $T \approx 800 K$ and a low temperature regime where correlated regions have a weaker JT-distorted symmetry., Comment: 4 pages, 4 Figures, submitted to PRL, new version with more data, text reformulated

In antiferromagnetic nanoparticles magnetization the linear component, $\chi_{AF}$H superposed to the saturation one usually complicates the fit of experimental data. We present a method based on scaling laws to determine the variation of $\chi_{AF}$ with temperature and to find the temperature dependence of the average magnetic moment $<\mu>$, without any assumption on both the magnetization dependence on field or the moment distribution function, whose relevance can also be estimated. We have applied this method to ferritin and found that $<\mu>$ decreases with increasing temperature and that a distribution function cannot be ignored. The fit with Langevin magnetization law and lognormal moment distribution functions yielded parameters close to those estimated with the scaling method. We also show that in general if the distribution is ignored, and a single particle moment $\mu_p$ is used, $\mu_p$ presents an artificial systematic increase with temperature. This calls the attention to the necessity of evaluating the effect of a size distribution before concluding about the physical nature of the parameters variation., Comment: Submitted to Phys. Rev. B

In the present work we analyze the influence of the charge-ordering on the magnetocaloric effect of Pr$_{1-x}$Ca$_x$MnO$_3$ manganites. The results for the samples with $x<$0.30 present the usual ferromagnetic behavior, peaking at the Curie temperature T$_C$. In contrast, for the samples above the onset concentration for the charge-ordering ($x\sim$0.30), an anomalous magnetic entropy change was observed below the charge-ordering temperature $T_{CO}$, persisting for lower temperatures. This effect is associated to a positive contribution to the magnetic entropy change due to charge-ordering, which is superimposed to the negative contribution from the spin ordering. We found that the charge-ordering component peaks at $T_N$ and is negligible above $T_{CO}$. Moreover, around T$^\star$ (temperature below which the insulator-metal transition induced by magnetic field becomes completely irreversible, where the system remains in such state even after the external magnetic field has been removed), we found extremely large values for the magnetic entropy change, establishing a `colossal' magnetocaloric effect on CMR manganites., Comment: Submitted to Phys. Rev. B

In the present paper we make a thorough analysis of a classical spin system, within the framework of Tsallis nonextensive statistics. From the analysis of the generalized Gibbs free energy, within the mean-field approximation, a para-ferromagnetic phase diagram, which exhibits first and second order phase transitions, is built. The features of the generalized, and classical, magnetic moment are mainly determined by the values of $q$, the non-extensive parameter. The model is successfully applied to the case of La$_{0.60}$Y$_{0.07}$Ca$_{0.33}$MnO$_3$ manganite. The temperature and magnetic field dependence of the experimental magnetization on this manganite are faithfully reproduced. The agreement between rather "exotic" magnetic properties of manganites and the predictions of the $q$-statistics, comes to support our early claim that these materials are magnetically nonextensive objects., Comment: 8 pages double column formatted + 13 figures. Submitted to Phys. Rev. B. Version 2 available to suppress technical problems with version 1

The low temperature behavior of Pr$_{1-x}$Ca$_{x}$MnO$_{3}$ manganites are known to undergo a transition at $x\sim$0.3, from an insulating ferromagnetic state, at low Ca concentration, to an insulating antiferromagnetic state. Above the onset concentration for the charge-ordering effect ($x\sim 0.3$), a metal-insulator transition induced by an external magnetic field is also observed and related to the collapse of the charge-ordered state. In this paper we show that the ferro-antiferromagnetic transition takes place in an inhomogeneous way: around the critical concentration the sample is a mixture of ferromagnetic and antiferromagnetic regions. The zero-field NMR measurements show that a fraction of the ferromagnetic regions is in a fast hopping regime, which suggests that a small fraction of the sample could be metallic, even in zero field. This fraction of fast hopping regions is maximal at $x=$0.3, which is also the concentration for which the insulator-metal transition has been observed in the smallest field., Comment: 4 pages, 4 figures. Submitted to Phys. Rev. B

We analyzed the magnetic behavior of a S-spin system within framework of the Tsallis nonextensive statistics, employing the normalized approach. Unusual properties on magnetization, entropy and susceptibility emerge, as a consequence of nonextensivity. We further show that the nonextensive approach can be relevant to the field of manganites, materials which exhibit long-range interactions and fractality, two basic ingredients for nonextensivity. Our results are in qualitative agreement to experimental data in La$_{0.67}$Ca$_{0.33}$MnO$_3$ and Pr$_{0.5}$Ca$_{0.5}$Mn$_{0.95}$Ga$_{0.05}$O$_3$ manganites., Comment: 5 pages and 6 figures. Submitted to Phys. Rev. B