An ultra-low field SQUID magnetometer for measuring antiferromagnetic and weakly remanent magnetic materials at low temperatures.

A novel setup for measuring magnetic fields of antiferromagnets (i.e., quadrupolar or higher-order magnetic fields) and generally weakly remanent magnetic materials is presented. The setup features a highly sensitive superconducting quantum interference device magnetometer with a magnetic field resolution of ∼ 10 fT and non-electric temperature control of the sample space for a temperature range of 1.5-65 K with a non-electric sample movement drive and optical position encoding. To minimize magnetic susceptibility effects, the setup components are degaussed and realized with plastic materials in sample proximity. Running the setup in magnetically shielded rooms allows for a well-defined ultra-low magnetic background field well below 150 nT in situ. The setup enables studies of inherently weak magnetic materials, which cannot be measured with high field susceptibility setups, optical methods, or neutron scattering techniques, giving new opportunities for the research on, e.g., spin-spiral multiferroics, skyrmion materials, and spin ices.

Tuning magnetoelectricity in a mixed-anisotropy antiferromagnet.

Control of magnetization and electric polarization is attractive in relation to tailoring materials for data storage and devices such as sensors or antennae. In magnetoelectric materials, these degrees of freedom are closely coupled, allowing polarization to be controlled by a magnetic field, and magnetization by an electric field, but the magnitude of the effect remains a challenge in the case of single-phase magnetoelectrics for applications. We demonstrate that the magnetoelectric properties of the mixed-anisotropy antiferromagnet LiNi1-xFexPO4 are profoundly affected by partial substitution of Ni2+ ions with Fe2+ on the transition metal site. This introduces random site-dependent single-ion anisotropy energies and causes a lowering of the magnetic symmetry of the system. In turn, magnetoelectric couplings that are symmetry-forbidden in the parent compounds, LiNiPO4 and LiFePO4, are unlocked and the dominant coupling is enhanced by almost two orders of magnitude. Our results demonstrate the potential of mixed-anisotropy magnets for tuning magnetoelectric properties.

Anomalous magnetic noise in an imperfectly flat landscape in the topological magnet Dy2Ti2O7.

Noise generated by motion of charge and spin provides a unique window into materials at the atomic scale. From temperature of resistors to electrons breaking into fractional quasiparticles, "listening" to the noise spectrum is a powerful way to decode underlying dynamics. Here, we use ultrasensitive superconducting quantum interference device (SQUIDs) to probe the puzzling noise in a frustrated magnet, the spin-ice compound Dy2Ti2O7 (DTO), revealing cooperative and memory effects. DTO is a topological magnet in three dimensions-characterized by emergent magnetostatics and telltale fractionalized magnetic monopole quasiparticles-whose real-time dynamical properties have been an enigma from the very beginning. We show that DTO exhibits highly anomalous noise spectra, differing significantly from the expected Brownian noise of monopole random walks, in three qualitatively different regimes: equilibrium spin ice, a "frozen" regime extending to ultralow temperatures, and a high-temperature "anomalous" paramagnet. We present several distinct mechanisms that give rise to varied colored noise spectra. In addition, we identify the structure of the local spin-flip dynamics as a crucial ingredient for any modeling. Thus, the dynamics of spin ice reflects the interplay of local dynamics with emergent topological degrees of freedom and a frustration-generated imperfectly flat energy landscape, and as such, it points to intriguing cooperative and memory effects for a broad class of magnetic materials.

Galvanic Replacement as a Synthetic Tool for the Construction of Anisotropic Magnetoplasmonic Nanocomposites with Synergistic Phototransducing and Magnetic Properties.

Magnetoplasmonic nanomaterials, which combine light and magnetic field responsiveness in an advantageous manner, are attractive candidates for bio-nanoapplications. However, the synthetic access to such hybrid particles has been limited by the incompatibility of the iron- and gold-based lattices. In this work, we provide the first insights into a new synthetic strategy for developing magnetoplasmonic anisotropic nanocomposites with prominent phototransducing properties. In our approach, magnetic nanocubes based on an alloy of iron oxide, zinc, and silver were constructed. In a key second stage, the galvanic replacement of silver with gold atoms yielded satellite-like magnetoplasmonic anisotropic structures. Superior magnetic and photoconverting properties were observed for the novel magnetoplasmonic nanocomposites when compared with the pure parent structures. Moreover, the synergy between the magnetic and optical stimuli was examined, showing shape-dependent contributions in the magnetization experiments. More importantly, an excellent cell ablation capability upon laser irradiation was observed for the magnetoplasmonic nanocomposites compared to the pure magnetic or plasmonic controls. Further demonstration of these novel theragnostic agents as MRI contrast agents is also reported even during the light-irradiation event. Thus, the described particles showed promising properties for bioapplications emerging from the novel synthetic methodology.

Revealing the NIR-triggered chemotherapy therapeutic window of magnetic and thermoresponsive nanogels.

The combination of magnetic nanoparticles and thermoresponsive nanogels represents an appealing strategy for the development of theranostic probes. These hybrid nanocarriers present several advantages such as outstanding properties for guided therapy, magnetic resonance imaging, and triggered release of encapsulated cargoes. Most magnetic thermoresponsive nanogels are built with strategies that comprise a physical interaction of particles with the polymeric network or the covalent attachment of a single particle to the linear polymer. Herein, we report a facile synthetic approach for the synthesis of magnetic and thermoresponsive nanogels that allows the controlled incorporation of multiple superparamagnetic inorganic cores as covalent cross-linkers. An ultrasonication-assisted precipitation-polymerization afforded nanogels with sizes in the nanometric range and similar magnetization and light transduction properties compared to the discrete magnetic nanoparticles. The theranostic capability of these nanocarriers was further investigated both in vitro and in vivo. In vivo experiments demonstrated the capacity of these materials as nanocarriers for near-infrared (NIR) triggered chemotherapy and highlighted the relevance of the correct concentration/dose in this antitumoral modality to achieve a superior therapeutic efficacy.

Ultralight magnetic aerogels from Janus emulsions.

Magnetite containing aerogels were synthesized by freeze-drying olive oil/silicone oil-based Janus emulsion gels containing gelatin and sodium carboxymethylcellulose (NaCMC). The magnetite nanoparticles dispersed in olive oil are processed into the gel and remain in the macroporous aerogel after removing the oil components. The coexistence of macropores from the Janus droplets and mesopores from freeze-drying of the hydrogels in combination with the magnetic properties offer a special hierarchical pore structure, which is of relevance for smart supercapacitors, biosensors, and spilled oil sorption and separation. The morphology of the final structure was investigated in dependence on initial compositions. More hydrophobic aerogels with magnetic responsiveness were synthesized by bisacrylamide-crosslinking of the hydrogel. The crosslinked aerogels can be successfully used in magnetically responsive clean up experiments of the cationic dye methylene blue.

Transferrin Decorated Thermoresponsive Nanogels as Magnetic Trap Devices for Circulating Tumor Cells.

A rational design of magnetic capturing nanodevices, based on a specific interaction with circulating tumor cells (CTCs), can advance the capturing efficiency and initiate the development of modern smart nanoformulations for rapid isolation and detection of these CTCs from the bloodstream. Therefore, the development and evaluation of magnetic nanogels (MNGs) based on magnetic nanoparticles and linear thermoresponsive polyglycerol for the capturing of CTCs with overexpressed transferrin (Tf(+) ) receptors has been presented in this study. The MNGs are synthesized using a strain-promoted "click" approach which has allowed the in situ surface decoration with Tf-polyethylene glycol (PEG) ligands of three different PEG chain lengths as targeting ligands. An optimal value of around 30% of cells captures is achieved with a linker of eight ethylene glycol units. This study shows the potential of MNGs for the capture of CTCs and the necessity of precise control over the linkage of the targeting moiety to the capturing device.

Solitonic lattice and Yukawa forces in the rare-earth orthoferrite TbFeO3.

The random fluctuations of spins give rise to many interesting physical phenomena, such as the 'order-from-disorder' arising in frustrated magnets and unconventional Cooper pairing in magnetic superconductors. Here we show that the exchange of spin waves between extended topological defects, such as domain walls, can result in novel magnetic states. We report the discovery of an unusual incommensurate phase in the orthoferrite TbFeO(3) using neutron diffraction under an applied magnetic field. The magnetic modulation has a very long period of 340 Å at 3 K and exhibits an anomalously large number of higher-order harmonics. These domain walls are formed by Ising-like Tb spins. They interact by exchanging magnons propagating through the Fe magnetic sublattice. The resulting force between the domain walls has a rather long range that determines the period of the incommensurate state and is analogous to the pion-mediated Yukawa interaction between protons and neutrons in nuclei.

Dipolar antiferromagnetism and quantum criticality in LiErF4.

Magnetism has been predicted to occur in systems in which dipolar interactions dominate exchange. We present neutron scattering, specific heat, and magnetic susceptibility data for LiErF(4), establishing it as a model dipolar-coupled antiferromagnet with planar spin-anisotropy and a quantum phase transition in applied field H(c|| = 4.0 ± 0.1 kilo-oersteds. We discovered non-mean-field critical scaling for the classical phase transition at the antiferromagnetic transition temperature that is consistent with the two-dimensional XY/h(4) universality class; in accord with this, the quantum phase transition at H(c) exhibits three-dimensional classical behavior. The effective dimensional reduction may be a consequence of the intrinsic frustrated nature of the dipolar interaction, which strengthens the role of fluctuations.