The competition of magnetic order and superconductivity is a key element in the physics of all unconventional superconductors, for example in high-transition-temperature cuprates, heavy fermions and organic superconductors. Here superconductivity is often found close to a quantum critical point where long-range antiferromagnetic order is gradually suppressed as a function of a control parameter, for example charge-carrier doping or pressure. It is believed that dynamic spin fluctuations associated with this quantum critical behaviour are crucial for the mechanism of superconductivity. Recently, high-temperature superconductivity has been discovered in iron pnictides, providing a new class of unconventional superconductors. Similar to other unconventional superconductors, the parent compounds of the pnictides show a magnetic ground state and superconductivity is induced on charge-carrier doping. In this Letter the structural and electronic phase diagram is investigated by means of X-ray scattering, muon spin relaxation and Mössbauer spectroscopy on the series LaO(1-x)F(x)FeAs. We find a discontinuous first-order-like change of the Néel temperature, the superconducting transition temperature and the respective order parameters. Our results strongly question the relevance of quantum critical behaviour in iron pnictides and prove a strong coupling of the structural orthorhombic distortion and the magnetic order both disappearing at the phase boundary to the superconducting state.

We present a detailed study on the magnetic order in the undoped mother compound LaFeAsO of the recently discovered Fe-based superconductor LaFeAsO1−xFx. In particular, we present local probe measurements of the magnetic properties of LaFeAsO by means of 57 Fe Mössbauer spectroscopy and muon spin relaxation in zero external field along with magnetization and resistivity studies. These experiments prove a commensurate static magnetic order with a strongly reduced ordered moment of 0.25(5) µB at the iron site below TN = 138 K, well separated from a structural phase transition at TS = 156 K. The temperature dependence of the sublattice magnetization is determined and compared to theory. Using a four-band spin density wave model both, the size of the order parameter and the quick saturation below TN are reproduced. PACS numbers: 76.75.+i, 76.80.+y, 75.30.Fv, The recently discovered Fe-based superconductors LaFeAsO 1−x F x [1] and the related materials in which La is substituted by Sm, Ce, Nd, Pr, and Gd, respectively [2,3,4,5,6,7] has triggered an intense research in the oxypnictides. Besides the high critical temperature above 50 K there are further striking similarities to the properties of the high-T C cuprates. The oxypnictides have a layered crystal structure with alternating FeAs and LaO sheets, where the Fe atoms are arranged on a simple square lattice [1]. Theoretical studies reveal a two-dimensional electronic structure [8] and it is believed that conductivity takes place mainly in the FeAs layers while the LaO layers provide the charge reservoir when doped with F ions. Again similar as in the cuprates, superconductivity emerges when doping a magnetic mother compound with electrons or holes and thereby supressing the magnetic order [9]. This suggests an interesting interplay between magnetism and superconductivity and, indeed, a recent theoretical work suggests that magnetic fluctuations associated with quantum critical point are essential for superconductivity in the electron doped LaFeAsO 1−x F x superconductors [10].However, in contrast to the cuprates, the magnetic mother compound is not a Mott-Hubbard insulator but a poor metal. A large covalency in the FeAs layers was found [8,11], which in the case of tetragonal LaFePO, i.e. the compound where As is replaced by P, leads to a non-magnetic ground state [12,13]. In contrast, in LaFeAsO there is an additional structural distortion at elevated temperatures [14,15] and a long range spin density wave (SDW) antiferromagnetic order has been observed in neutron scattering experiments on powder samples below ∼150 K. [15]. First principle calculations yield antiferromagnetic order with Fe magnetic moments ranging from 1.5 µ B to 2.3 µ B [10,16,17,18], while the neutron scattering experiments indicate a much smaller value. Assuming that the full sample volume is contributing to the magnetic scattering an ordered moment of ∼ 0.35 µ B [15] is inferred from the weak superlattice reflections in powder neutron diffraction. A local probe measurement, which could verify...

Nickel ferrite (NiFe2O4) nanoparticles with an average crystallite size of about 8.6 nm were prepared by mechanochemical synthesis (mechanosynthesis). In-field Mössbauer spectroscopy and high-resolution TEM studies revealed a nonuniform structure of mechanosynthesized NiFe2O4 nanoparticles consisting of an ordered core surrounded by a disordered grain boundary (surface) region. The inner core of a NiFe2O4 nanoparticle is considered to possess a fully inverse spinel structure with a Néel-type collinear spin alignment, whereas the surface shell is found to be structurally and magnetically disordered due to the nearly random distribution of cations and the canted spin arrangement. As a consequence of frustrated superexchange interactions in the surface shell, the mechanosynthesized NiFe2O4 exhibits a reduced nonsaturating magnetization, an enhanced coercivity, and a shifted hysteresis loop. The study also demonstrates that one can tailor the magnetic properties of mechanosynthesized NiFe2O4 particles by suitably controlling their size. The thickness of the surface shell of about 1 nm estimated from size-dependent magnetization measurements is found to be in good agreement with that obtained from high-resolution TEM and Mössbauer experiments. On heating above 673 K, the mechanosynthesized NiFe2O4 relaxes to a structural and magnetic state that is similar to the bulk one.

The magnetic properties of monodisperse FeO-Fe3O4 nanoparticles with different mean sizes and volume fractions of FeO synthesized via decomposition of iron oleate were correlated to their crystallographic and phase compositional features by exploiting high resolution transmission electron microscopy, X-ray diffraction, Mössbauer spectroscopy and field and zero field cooled magnetization measurements. A model describing the phase transformation from a pure Fe3O4 phase to a mixture of Fe3O4, FeO and interfacial FeO-Fe3O4 phases as the particle size increases was established. The reduced magnetic moment in FeO-Fe3O4 nanoparticles was attributed to the presence of differently oriented Fe3O4 crystalline domains in the outer layers and paramagnetic FeO phase. The exchange bias energy, dominating magnetization reversal mechanism and superparamagnetic blocking temperature in FeO-Fe3O4 nanoparticles depend strongly on the relative volume fractions of FeO and the interfacial phase.

A quantum spin liquid state has long been predicted to arise in spin-1/2 Heisenberg square-lattice antiferromagnets at the boundary region between Néel (nearest-neighbor interaction dominates) and columnar (next-nearest-neighbor interaction dominates) antiferromagnetic order. However, there are no known compounds in this region. Here we use d10–d0 cation mixing to tune the magnetic interactions on the square lattice while simultaneously introducing disorder. We find spin-liquid-like behavior in the double perovskite Sr2Cu(Te0.5W0.5)O6, where the isostructural end phases Sr2CuTeO6 and Sr2CuWO6 are Néel and columnar type antiferromagnets, respectively. We show that magnetism in Sr2Cu(Te0.5W0.5)O6 is entirely dynamic down to 19 mK. Additionally, we observe at low temperatures for Sr2Cu(Te0.5W0.5)O6—similar to several spin liquid candidates—a plateau in muon spin relaxation rate and a strong T-linear dependence in specific heat. Our observations for Sr2Cu(Te0.5W0.5)O6 highlight the role of disorder in addition to magnetic frustration in spin liquid physics.

A single-step synthesis of magnesium ferrite (MgFe 2 O 4 ) nanoparticles with an average crystallite size of about 8.5 nm synthesized via mechanochemical processing of binary oxide precursors at room temperature is reported. The study highlights the nature of the cation disorder and of the spin arrangement in mechanosynthesized MgFe 2 O 4 as well as its response to changes in temperature. An unusual property of the magnetization enhancement in nanoscale mechanosynthesized MgFe 2 O 4 is reported. Whereas the inner core of a MgFe 2 O 4 nanoparticle exhibits a partly inverse spinel structure with a Ne ´el type collinear spin alignment, the major features of the ionic and spin configurations in the grain boundary (surface) region are a nonequilibrium cation distribution and a canted spin arrangement. Although the spin-canting effect tends to reduce the magnetic moment, the magnetization enhancement exhibited by mechanosynthesized MgFe 2 O 4 is attributed to the nearly random distribution of magnetic cations in the surface regions of nanoparticles. On heating above 623 K, the mechanosynthesized MgFe 2 O 4 relaxes to a structural and magnetic state that is similar to the bulk one.

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Herein, by studying a stepwise phase transformation of 23 nm FeO-Fe3O4 core-shell nanocubes into Fe3O4, we identify a composition at which the magnetic heating performance of the nanocubes is not affected by the medium viscosity and aggregation. Structural and magnetic characterizations reveal the transformation of the FeO-Fe3O4 nanocubes from having stoichiometric phase compositions into Fe 2+ deficient Fe3O4 phases. The resultant nanocubes contain tiny compressed and randomly distributed FeO sub-domains as well as structural defects. This phase transformation causes a tenfold increase in the magnetic losses of the nanocubes, which remains exceptionally insensitive to the medium viscosity as well as aggregation unlike similarly sized single-phase magnetite nanocubes. We observe that the dominant relaxation mechanism switches from Néel in fresh core-shell nanocubes to Brownian in partially oxidized nanocubes and once again to Néel in completely treated nanocubes. The Fe 2+ deficiencies and structural defects appear to reduce the magnetic energy barrier and anisotropy field, thereby driving the overall relaxation into Néel process. The magnetic losses of the particles remain unchanged through a progressive internalization/association to ovarian cancer cells. Moreover, the particles induce a significant cell death after being exposed to hyperthermia treatment. Here, we present the largest heating performance that has been reported to date for 23 nm iron oxide nanoparticles under cellular and intracellular conditions. Our findings clearly demonstrate the positive impacts of the Fe 2+ deficiencies and structural defects in the Fe3O4 structure on the heating performance under cellular and intracellular conditions.