Magnetic structure factor of correlated moments in small-angle neutron scattering

The interplay between structural and magnetic properties of nanostructured magnetic materials allows one to realize unconventional magnetic effects, which results in a demand for experimental techniques to determine the magnetization profile with nanoscale resolution. Magnetic small-angle neutron scattering (SANS) probes both the chemical and magnetic nanostructure and is thus a powerful technique, e.g., for the characterization of magnetic nanoparticles. Here, we show that the conventionally used particle-matrix approach to describe SANS of magnetic particle assemblies, however, leads to a flawed interpretation. As a remedy, we provide general expressions for the field-dependent two-dimensional magnetic SANS cross section of correlated moments. It is shown that for structurally disordered ensembles the magnetic structure factor is in general, and contrary to common assumptions, (i) anisotropic also in zero field and (ii) that even in saturation the magnetic structure factor deviates from the nuclear one. These theoretical predictions explain qualitatively the intriguing experimental, polarized SANS data of an ensemble of dipolar-coupled iron oxide nanoparticles.This project has received funding from the European Commission Framework Programme 7 under Grant Agreement No. 604448 (NanoMag)

Supraferromagnetic correlations in clusters of magnetic nanoflowers

Magnetic nanoflowers are densely packed aggregates of superferromagnetically coupled iron oxide nanocrystallites, which excel during magnetic hyperthermia experiments. Here, we investigate the nature of the moment coupling within a powder of such nanoflowers using spin-resolved small-angle neutron scattering. Within the powder, the nanoparticles are agglomerated to clusters, and we can show that the moments of neighboring nanoflowers tend to align parallel to each other. Thus, the whole system resembles a hierarchical magnetic nanostructure consisting of three distinct levels, i.e., (i) the ferrimagnetic nanocrystallites as building blocks, (ii) the superferromagnetic nanoflowers, and (iii) the supraferromagnetic clusters of nanoflowers. We surmise that such a supraferromagnetic coupling explains the enhanced magnetic hyperthermia performance in the case of interacting nanoflowers.This project received funding from the European Commission Framework Programme 7 under Grant Agreement No. 604448 (NanoMag), the National Research Fund of Luxembourg (No. CORE SANS4NCC Grant), and the Spanish Government (No. MAT2017-83631-C3-R)

Nonlinear susceptibilities as a probe to unambiguously distinguish between canonical and cluster spin glasses

Treating the randomly Fe-substituted optimally hole-doped manganite La0.7Pb0.3(Mn1−yFey)O3 (y=0.2,0.3) as a test case, we demonstrate that a combined investigation of both odd and even harmonics of the ac magnetic response permits an unambiguous distinction between the canonical and cluster spin glasses. As expected for a spin glass (SG), the nonlinear ac magnetic susceptibilities χ3(T,ω) and χ5(T,ω) (odd armonics) diverge at the SG freezing temperature Tg=80.00(3) K [Tg=56.25(5) K] in the static limit and, like the imaginary part of the linear susceptibility, follow dynamic scaling with the critical exponents β=0.56(3) [β=0.63(3)], γ=1.80(5) [γ=2.0(1)], and zν=10.1(1) [zν=8.0(5)] in the sample with composition y=0.2 (y=0.3). The nonlinear susceptibility χNL, which has contributions from both χ3 and χ5, satisfies static scaling with the same choice of Tg, β, and γ. Irrespective of the Fe concentration, the values of the critical exponents γ, ν, and η are in much better agreement with those theoretically predicted for a three-dimensional (d=3) Heisenberg chiral SG than for a d=3 Ising SG. The true thermodynamic nature of the “zero-field” spin-glass transition is preserved even in finite magnetic fields. Unlike odd harmonics, even harmonics χ2(T,ω) and χ4(T,ω) make it evident that, apart from the macroscopic length scale of the spin-glass order in the static limit, there exists a length scale that corresponds to the short-range ferromagnetic order.This work was supported by the Department of Science and Technology, India, through Grant No. IR/S5/IU-01/2006, and by the Spanish Ministry for Education through the grant No. SAB 2010-0091. S.N.K. is thankful to the Department of Science and Technology, India, for financial support through the J. C. Bose National Fellowship. Y.B. thanks the Council for Scientific and Industrial Research, India, for the financial support through a Senior Research Fellowship. The authors thank J. M. Barandiaran and J. Gutiérrez for providing the samples

Condiciones de vida en las cuencas mineras centrales de Asturias durante la fase expansiva de la revolución industrial asturiana (1885-1907) a través de las Topografías Médicas

En este artículo exponemos las duras condiciones de vida de los obreros minero-metalúrgicos de las cuencas mineras del Nalón y del Caudal-Aller analizando las Topografías Médicas en el momento de expansión de la revolución industrial asturiana. El sistema básico de supervivencia estaba plagado de anomalías que se justifican por el escaso rendimiento fabril debido a los «obreros mixtos». Aspecto que no se pudo resolver con las ayudas empresariales que ofrecía el «pensamiento paternalista»

Observation of isotropic-dipolar to isotropic-Heisenberg crossover in Co-and Ni-substituted manganites

High-precision ac susceptibility data have been taken on the La0.7Pb0.3Mn1?y (Co, Ni)yO3 (y = 0, 0.1, 0.2 and 0.3) manganite system over a wide range of amplitudes and frequencies of the ac driving field in a temperature range that embraces the critical region near the ferromagnetic (FM)?paramagnetic (PM) phase transition (occurring at the Curie point TC). Elaborate data analysis was performed that (i) enabled the first observation of a crossover from a three-dimensional (3D; d = 3) isotropic long-range dipolar asymptotic critical behavior to a d = 3 isotropic short-range Heisenberg critical regime as the temperature is raised from TC in the compositions y 6= 0 (no such crossover is observed in the parent compound, y = 0) and (ii) brought out clearly the importance of dipole?dipole interactions between the eg electron spins and/or between eg?t2g electron spins in establishing long-range FM order in the insulating state. The final charge and spin states of Co and Ni ions, substituting for the Mn3+ and/or Mn4+ ions, are arrived at by using a scenario of substitution that is consistent not only with the present results but also with the previously published structural, thermo-gravimetric, bulk magnetization, dc magnetic susceptibility and electrical resistivity data on the same system. The marked similarity seen between the magnetic behavior of the manganite system in question and the quenched random-exchange ferromagnets, within and outside the critical region, suggests that the percolation model forms an adequate description of the FM metal-to-PM insulator transition

Influence of data sources and processing methods on theoretical river network quality

ABSTRACT: Stream ecosystem research and water resource management need to be considered over broad spatial scales. Moreover, the investigation of the spatial configuration and habitat characteristics of streams requires an accurate and precise spatial framework to reflect a catchment's physical reality that can successfully explain observed patterns at smaller scales. In this sense, geographic information systems represent an essential tool to satisfy the needs of researchers and managers. Specifically, theoretical river networks (TRNs) extracted from digital elevation models (DEMs) have become much more common in recent years, as they can provide a suitable spatial network and hierarchical organisation to sort out river ecosystem information from reach to catchment levels. Nevertheless, the quality of the extracted TRN depends greatly on the spatial resolution of the DEM and the methodology used in the network extraction processes. In this study, we compare the quality of 9 TRNs extracted from DEMs with different spatial resolutions ranging from regional (5 m) to national (25 m) and global scales (90 m) using the ArcHydro, Hec-GeoHMS and Netstream software packages. To achieve our goal, we compared (i) the DEM-derived slope; (ii) the spatial accuracy of the TRNs in relation to a control river network; (iii) the structure of the TRNs through analysis of the number of river segments, average river segment length and total river length by stream order, drainage density and the mean upstream slope throughout the TRN; and (iv) the ability of variables derived from TRNs to discriminate among stream types classified according to flow type and substrate composition. We demonstrated that not only DEM spatial resolution but also the DEM data source and raster creation process exert an important influence on terrain characteristics derived from DEMs and TRN properties. Moreover, TRNs extracted with NetStream generally showed better performance than those extracted with ArchHydro and HecGeoHMS. Nevertheless, river network extraction quality, DEM spatial resolution and extraction algorithms exhibit complex relationships due to the large number of interacting factors.The work described in this paper is part of a research project financed by the National Plan (2008-2011) for Research in Science & Technology of the Spanish Government (Project CTM2009-07447). The authors appreciate the valuable suggestions of anonymous reviewers that greatly improvement the document

Influence of data sources and processing methods on theoretical river network quality

Stream ecosystem research and water resource management need to be considered over broad spatial scales. Moreover, the investigation of the spatial configuration and habitat characteristics of streams requires an accurate and precise spatial framework to reflect a catchment's physical reality that can successfully explain observed patterns at smaller scales. In this sense, geographic information systems represent an essential tool to satisfy the needs of researchers and managers. Specifically, theoretical river networks (TRNs) extracted from digital elevation models (DEMs) have become much more common in recent years, as they can provide a suitable spatial network and hierarchical organisation to sort out river ecosystem information from reach to catchment levels. Nevertheless the quality of the extracted TRN depends greatly on the spatial resolution of the DEM and the methodology used in the network extraction processes. In this study, we compare the quality of 9 TRNs extracted from DEMs with different spatial resolutions ranging from regional (5 m) to national (25 m) and global scales (90 m) using the ArcHydro, Hec-GeoHMS and Netstream software packages. To achieve our goal, we compared (i) the DEM-derived slope; (ii) the spatial accuracy of the TRNs in relation to a control river network; (iii) the structure of the TRNs through analysis of the number of river segments, average river segment length and total river length by stream order, drainage density and the mean upstream slope throughout the TRN; and (iv) the ability of variables derived from TRNs to discriminate among stream types classified according to flow type and substrate composition. We demonstrated that not only DEM spatial resolution but also the DEM data source and raster creation process exert an important influence on terrain characteristics derived from DEMs and TRN properties. Moreover, TRNs extracted with NetStream generally showed better performance than those extracted with ArchHydro and HecGeoHMS. Nevertheless, river network extraction quality, DEM spatial resolution and extraction algorithms exhibit complex relationships due to the large number of interacting factors.La investigación de los ecosistemas acuáticos continentales y la gestión de recursos hídricos necesitan ser considerados a escalas espaciales que abarquen grandes territorios. Así mismo, el estudio de la configuración espacial de los sistemas fluviales y las características del hábitat requieren de un marco espacial preciso con el que explicar los patrones observados a pequeña escala a partir de las características físicas de la cuenca. En este sentido, los sistemas de información geográfica representan una herramienta esencial. Específicamente, la extracción de redes fluviales teóricas (RFT) a partir de modelos digitales de elevación (MDEs) ha sufrido una importante expansión y desarrollo en los últimos años. Las RTF, proporcionan un marco espacial adecuado e integran la estructura jerárquica de los ecosistemas fluviales, de tal modo que pueden englobar información a diferentes escales espaciales, desde el nivel de cuenca al de tramo. Sin embargo, la calidad de las RFTs depende, en gran medida, de la resolución espacial de los MDE y de los métodos utilizados en el proceso de extracción de la red. En este estudio hemos comparado la calidad de 9 RFTs obtenidas a partir de MDEs con diferentes resoluciones espaciales, que van desde la escala regional (5 m), nacional (25 m) hasta global (90 m) mediante ArcHydro, HecGeoHMS y NetStream.Para lograr nuestro objetivos hemos comparado (i) las características de la pendiente derivada de los MDEs, (ii) la precisión espacial de las RFT en relación a una red fluvial control, (iii) la estructura de los RTFs mediante el análisis del número de segmentos, la longitud media y total de los segmentos de cada orden fluvial, la densidad de drenaje y la pendiente media de la cuenca a lo largo de la RFT y (iv) la capacidad de variables físicas derivadas de las RFT para discriminar entre tipos de ríos clasificados con base en el tipo de flujo y la composición del sustrato. Los resultados obtenidos han demostrado que la calidad de las características físicas derivadas del MDE y las propiedades de las RFTs no están determinadas únicamente por la resolución espacial del MDE, sino que el tipo de dato del que provenga el MDE y el proceso de generación del mismo ejercen una gran influencia. Además, NetStream ha generado, por lo general, unas RTFs más precisas que ArcHydro y HecGeoHMS. Sin embargo, la interacción de un gran número de factores durante el proceso de generación de redes hace que las relaciones entre la calidad de las mismas, la resolución espacial de los MDE y los algoritmos utilizados sean complejas

Dipolar-coupled moment correlations in clusters of magnetic nanoparticles

Here, we investigate the nature of the moment coupling between 10-nm DMSA-coated magnetic nanoparticles, in both colloidal dispersion and in powder form. The individual iron oxide cores were composed of > 95% maghemite and agglomerated to clusters. At room temperature the ensemble behaved as a superparamagnet according to M\"ossbauer and magnetization measurements, however, with clear signs of dipolar interactions at low temperatures. Analysis of temperature-dependent AC susceptibility data in the superparamagnetic regime indicates a tendency for dipolar coupled anticorrelations of the core moments within the clusters. To resolve the directional correlations between the particle moments we performed polarized small-angle neutron scattering and determined the magnetic spin-flip cross-section of the powder in low magnetic field at 300 K. We extract the underlying pair distance distribution function of the magnetization vector field by an indirect Fourier transform of the cross-section, and which suggests positive as well as negative correlations between nearest neighbor moments, with anticorrelations clearly dominating for next-nearest moments. These tendencies are confirmed by Monte Carlo simulations of such core-clusters.Comment: 11 pages, 6 figure

Crossover from superspin glass to superferromagnet in FexAg100-x nanostructured thin films ( 20 ≤ x ≤ 50 )

FexAg100?x granular thin films, with 20 x 50, have been prepared by the dc-magnetron sputtering deposition technique. With this technique we have been able to obtain samples comprising small Fe nanoparticles 2.5?3 nm embedded in a Ag matrix, remaining their size practically constant with increasing Fe content. Their magnetic behavior has been fully characterized by dc magnetic measurements between 5?350 K. They have revealed a crossover in the collective magnetic behavior of the Fe nanoparticles around a 35 at. %. Below such a concentration, a collective freezing of the magnetic moments is observed at low temperatures, while at high temperatures a transition, mainly mediated by dipolar interactions, to a magnetically disordered state is obtained. Above this concentration, direct exchange interactions overcome the dipolar magnetic interactions and a long-range order tends to prevail in the range of temperatures analyzed. ac magnetic measurements have indicated a crossover from a superspin glass x35 to a superferromagnetic x35 behavior for the magnetic moments of the Fe nanoparticles.This work was supported by the CICYT of Spain under Contracts No. MAT2008-06542-C04-02 and No. MAT2008- 06542-C04-04. SGIker technical support MEC, GV/EJ, European Social Fund is gratefully acknowledged. The financial support from the Basque Government Department of Education Project No. IT-347-07 is acknowledged

Modifying the magnetic response of magnetotactic bacteria: incorporation of Gd and Tb ions into the magnetosome structure

Magnetotactic bacteria Magnetospirillum gryphiswaldense MSR-1 biosynthesise chains of cube–octahedral magnetosomes, which are 40 nm magnetite high quality (Fe3O4) nanoparticles. The magnetic properties of these crystalline magnetite nanoparticles, which can be modified by the addition of other elements into the magnetosome structure (doping), are of prime interest in a plethora of applications, those related to cancer therapy being some of the most promising ones. Although previous studies have focused on transition metal elements, rare earth (RE) elements are very interesting as doping agents, both from a fundamental point of view (e.g. significant differences in ionic sizes) and for the potential applications, especially in biomedicine (e.g. magnetic resonance imaging and luminescence). In this work, we have investigated the impact of Gd and Tb on the magnetic properties of magnetosomes by using different complementary techniques. X-ray diffraction, transmission electron microscopy, and X-ray absorption near edge spectroscopy analyses have revealed that a small amount of RE ions, ∼3–4%, incorporate into the Fe3O4 structure as Gd3+ and Tb3+ ions. The experimental magnetic characterisation has shown a clear Verwey transition for the RE-doped bacteria, located at T ∼ 100 K, which is slightly below the one corresponding to the undoped ones (106 K). However, we report a decrease in the coercivity and remanence of the RE-doped bacteria. Simulations based on the Stoner–Wohlfarth model have allowed us to associate these changes in the magnetic response with a reduction of the magnetocrystalline (KC) and, especially, the uniaxial (Kuni) anisotropies below the Verwey transition. In this way, Kuni reaches a value of 23 and 26 kJ m−3 for the Gd- and Tb-doped bacteria, respectively, whilst a value of 37 kJ m−3 is obtained for the undoped bacteria.This work was supported in part by the Spanish MCIN/AEI under Projects MAT2017-83631-C3-R and PID2020-115704RB-C33. The work of Elizabeth M. Jefremovas was supported by the “Concepción Arenal Grant” awarded by Gobierno de Cantabria and Universidad de Cantabria. The work of Lourdes Marcano was supported by the Postdoctoral Fellowship from the Basque Government under Grant POS-2019-2-0017. The authors would like to thank “Nanotechnology in translational hyperthermia” (HIPERNANO)-RED2018-102626-T. We thank the ALBA (CLAESS beamline) synchrotron radiation facilities and staff for the allocation of beamtime and assistance during the experiments