Experimental probing of exchange interactions between localized spins in the dilute magnetic insulator (Ga,Mn)N

The sign, magnitude, and range of the exchange couplings between pairs of Mn ions is determined for (Ga,Mn)N and (Ga,Mn)N:Si with x < 3%. The samples have been grown by metalorganic vapor phase epitaxy and characterized by secondary-ion mass spectroscopy; high-resolution transmission electron microscopy with capabilities allowing for chemical analysis, including the annular dark-field mode and electron energy loss spectroscopy; high-resolution and synchrotron x-ray diffraction; synchrotron extended x-ray absorption fine-structure; synchrotron x-ray absorption near-edge structure; infra-red optics and electron spin resonance. The results of high resolution magnetic measurements and their quantitative interpretation have allowed to verify a series of ab initio predictions on the possibility of ferromagnetism in dilute magnetic insulators and to demonstrate that the interaction changes from ferromagnetic to antiferromagnetic when the charge state of the Mn ions is reduced from 3+ to 2+.Comment: 12 pages, 14 figures; This version contains the detailed characterization of the crystal structure as well as of the Mn distribution and charge stat

Paramagnetic GaN:Fe and ferromagnetic (Ga,Fe)N - relation between structural, electronic, and magnetic properties

We report on the metalorganic chemical vapor deposition (MOCVD) of GaN:Fe and (Ga,Fe)N layers on c-sapphire substrates and their thorough characterization via high-resolution x-ray diffraction (HRXRD), transmission electron microscopy (TEM), spatially-resolved energy dispersive X-ray spectroscopy (EDS), secondary-ion mass spectroscopy (SIMS), photoluminescence (PL), Hall-effect, electron-paramagnetic resonance (EPR), and magnetometry employing a superconducting quantum interference device (SQUID). A combination of TEM and EDS reveals the presence of coherent nanocrystals presumably FexN with the composition and lattice parameter imposed by the host. From both TEM and SIMS studies, it is stated that the density of nanocrystals and, thus the Fe concentration increases towards the surface. In layers with iron content x<0.4% the presence of ferromagnetic signatures, such as magnetization hysteresis and spontaneous magnetization, have been detected. We link the presence of ferromagnetic signatures to the formation of Fe-rich nanocrystals, as evidenced by TEM and EDS studies. This interpretation is supported by magnetization measurements after cooling in- and without an external magnetic field, pointing to superparamagnetic properties of the system. It is argued that the high temperature ferromagnetic response due to spinodal decomposition into regions with small and large concentration of the magnetic component is a generic property of diluted magnetic semiconductors and diluted magnetic oxides showing high apparent Curie temperature.Comment: 21 pages, 30 figures, submitted to Phys. Rev.

Machine Learning May Sometimes Simply Capture LiteraturePopularity Trends: A Case Study of Heterocyclic Suzuki-MiyauraCoupling br

Applications of machine learning (ML) to synthetic chemistry rely on the assumption that large numbers ofliterature-reported examples should enable construction of accurate and predictive models of chemical reactivity. This paperdemonstrates that abundance of carefully curated literature data may be insufficient for this purpose. Using an example of Suzuki-Miyaura coupling with heterocyclic building blocks &amp; xe0d5;and a carefully selected database of &gt;10,000 literature examples &amp; xe0d5;we show thatML models cannot offer any meaningful predictions of optimum reaction conditions, even if the search space is restricted to onlysolvents and bases. This result holds irrespective of the ML model applied (from simple feed-forward to state-of-the-art graph-convolution neural networks) or the representation to describe the reaction partners (variousfingerprints, chemical descriptors,latent representations, etc.). In all cases, the ML methods fail to perform significantly better than naive assignments based on thesheer frequency of certain reaction conditions reported in the literature. These unsatisfactory results likely reflect subjectivepreferences of various chemists to use certain protocols, other biasing factors as mundane as availability of certain solvents/reagents,and/or a lack of negative data. Thesefindings highlight the likely importance of systematically generating reliable and standardizeddata sets for algorithm training

Identification of blood biomarkers of rheumatoid arthritis by transcript profiling of peripheral blood mononuclear cells from the rat collagen-induced arthritis model

Rheumatoid arthritis (RA) is a chronic debilitating autoimmune disease that results in joint destruction and subsequent loss of function. To better understand its pathogenesis and to facilitate the search for novel RA therapeutics, we profiled the rat model of collagen-induced arthritis (CIA) to discover and characterize blood biomarkers for RA. Peripheral blood mononuclear cells (PBMCs) were purified using a Ficoll gradient at various time points after type II collagen immunization for RNA preparation. Total RNA was processed for a microarray analysis using Affymetrix GeneChip technology. Statistical comparison analyses identified differentially expressed genes that distinguished CIA from control rats. Clustering analyses indicated that gene expression patterns correlated with laboratory indices of disease progression. A set of 28 probe sets showed significant differences in expression between blood from arthritic rats and that from controls at the earliest time after induction, and the difference persisted for the entire time course. Gene Ontology comparison of the present study with previous published murine microarray studies showed conserved Biological Processes during disease induction between the local joint and PBMC responses. Genes known to be involved in autoimmune response and arthritis, such as those encoding Galectin-3, Versican, and Socs3, were identified and validated by quantitative TaqMan RT-PCR analysis using independent blood samples. Finally, immunoblot analysis confirmed that Galectin-3 was secreted over time in plasma as well as in supernatant of cultured tissue synoviocytes of the arthritic rats, which is consistent with disease progression. Our data indicate that gene expression in PBMCs from the CIA model can be utilized to identify candidate blood biomarkers for RA

Controlling Curie temperature in (Ga,Ms)As through location of the Fermi level within the impurity band

The ferromagnetic semiconductor (Ga,Mn)As has emerged as the most studied material for prototype applications in semiconductor spintronics. Because ferromagnetism in (Ga,Mn)As is hole-mediated, the nature of the hole states has direct and crucial bearing on its Curie temperature TC. It is vigorously debated, however, whether holes in (Ga,Mn)As reside in the valence band or in an impurity band. In this paper we combine results of channeling experiments, which measure the concentrations both of Mn ions and of holes relevant to the ferromagnetic order, with magnetization, transport, and magneto-optical data to address this issue. Taken together, these measurements provide strong evidence that it is the location of the Fermi level within the impurity band that determines TC through determining the degree of hole localization. This finding differs drastically from the often accepted view that TC is controlled by valence band holes, thus opening new avenues for achieving higher values of TC.Comment: 5 figures, supplementary material include

Cytotoxic lymphocytes in B-cell chronic lymphocytic leukemia

The occurrence of cytotoxic lymphocyte subpopulations (i.e., CD 16+, CD57+ and cytotoxic CD 8+) was studied in the peripheral blood of 18 B-cell chronic lymphocytic leukemia (B-CLL) patients. The absolute numbers of CD 57+, CD 16+ and cytotoxic CD 8+ lymphocytes were increased in the peripheral blood of untreated patients as compared with healthy donors, suggesting a causal relation with the accumulation of malignant B-cells. For 5 B-CLL patients and 5 hematological normal donors, the lymphocyte subpopulations in peripheral blood, lymph nodes and bone marrow were determined. A significant immune response was observed in the lymph nodes of the patients, as reflected by the CD 3+ lymphocytes, which were 1.7–27 times larger in the patients lymph nodes than in their peripheral blood and bone marrow. In contrast, with peripheral blood this was mainly caused by an increase in CD 4+ lymphocytes. The CD 57 lymphocytes in the lymph nodes of the patients had abnormal orthogonal light-scattering signals and an abnormal density of CD 57+ receptors in comparison with their peripheral blood CD 57+ lymphocytes or the CD57+ lymphocytes in the peripheral blood, bone marrow and tonsils of the hematological normal donors. This study shows that although a significant increase of cytotoxic lymphocytes in the peripheral blood of B-CLL patients is observed, the actual distributions of the non-malignant lymphocytes can be quite different at the actual tumor sites, i.e., bone marrow and lymph node

Microplastic in angling baits as a cryptic source of contamination in European freshwaters.

High environmental microplastic pollution, and its largely unquantified impacts on organisms, are driving studies to assess their potential entry pathways into freshwaters. Recreational angling, where many anglers release manufactured baits into freshwater ecosystems, is a widespread activity with important socio-economic implications in Europe. It also represents a potential microplastic pathway into freshwaters that has yet to be quantified. Correspondingly, we analysed three different categories of industrially-produced baits ('groundbait', 'boilies' and 'pellets') for their microplastic contamination (particles 700 µm to 5 mm). From 160 samples, 28 microplastics were identified in groundbait and boilies, with a mean concentration of 17.4 (± 48.1 SD) MP kg-1 and 6.78 (± 29.8 SD) mg kg-1, yet no microplastics within this size range were recorded in the pellets. Microplastic concentrations significantly differed between bait categories and companies, but microplastic characteristics did not vary. There was no correlation between microplastic contamination and the number of bait ingredients, but it was positively correlated with C:N ratio, indicating a higher contamination in baits with higher proportion of plant-based ingredients. We thus reveal that bait microplastics introduced accidentally during manufacturing and/or those originating from contaminated raw ingredients might be transferred into freshwaters. However, further studies are needed to quantify the relative importance of this cryptic source of contamination and how it influences microplastic levels in wild fish