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Growth, electrical, structural, and magnetic properties of half-Heusler CoT i 1 - x F e x Sb
Epitaxial thin films of the substitutionally alloyed half-Heusler series CoTi 1-x Fe x Sb were grown by molecular beam epitaxy on InAlAs/InP(001) substrates for concentrations 0.0 ≤ x ≤ 1.0. The influence of Fe on the structural, electronic, and magnetic properties was studied and compared to that expected from density functional theory. The films are epitaxial and single crystalline, as measured by reflection high-energy electron diffraction and X-ray diffraction. Using in-situ X-ray photoelectron spectroscopy, only small changes in the valence band are detected for x ≤ 0.5. For films with x ≥ 0.05, ferromagnetism is observed in SQUID magnetometry with a saturation magnetization that scales linearly with Fe content. A dramatic decrease in the magnetic moment per formula unit occurs when the Fe is substitutionally alloyed on the Co site indicating a strong dependence on the magnetic moment with site occupancy. A crossover from both in-plane and out-of-plane magnetic moments to only in-plane moment occurs for higher concentrations of Fe. Ferromagnetic resonance indicates a transition from weak to strong interaction with a reduction in inhomogeneous broadening as Fe content is increased. Temperature-dependent transport reveals a semiconductor to metal transition with thermally activated behavior for x ≤ 0.5. Anomalous Hall effect and large negative magnetoresistance (up to -18.5% at 100 kOe for x=0.3) are observed for higher Fe content films. Evidence of superparamagnetism for x=0.3 and x=0.2 suggests for moderate levels of Fe, demixing of the CoTi 1-x Fe x Sb films into Fe rich and Fe deficient regions may be present. Atom probe tomography is used to examine the Fe distribution in a x=0.3 film. Finally, statistical analysis reveals a nonhomogeneous distribution of Fe atoms throughout the film, which is used to explain the observed magnetic and electrical behavior.
Optimizing Magnetite Nanoparticles for Mass Sensitivity in Magnetic Particle Imaging
Purpose: Magnetic particle imaging (MPI), using magnetite nanoparticles (MNPs) as tracer material, shows great promise as a platform for fast tomographic imaging. To date, the magnetic properties of MNPs used in imaging have not been optimized. As nanoparticle magnetism shows strong size dependence, we explore how varying MNP size impacts imaging performance in order to determine optimal MNP characteristics for MPI at any driving field frequency f 0 . Methods: Monodisperse MNPs of varying size were synthesized and their magnetic properties characterized. Their MPI response was measured experimentally, at an arbitrarily chosen f 0 = 250 kHz, using a custom-built MPI transceiver designed to detect the third harmonic of MNP magnetization. Results were interpreted using a model of dynamic MNP magnetization that is based on the Langevin theory of superparamagnetism and accounts for sample size distribution, and size-dependent magnetic relaxation. Results: Our experimental results show clear variation in the MPI signal intensity as a function of MNP size that is in good agreement with modeled results. A maxima in the plot of MPI signal vs. MNP size indicates there is a particular size that is optimal for the chosen frequency of 250 kHz. Conclusions: For MPI at any chosen frequency, there will exist a characteristic particle size that generates maximum signal amplitude. We illustrate this at 250 kHz with particles of 15 nm core diameter.
Structure and magnetoresistance of a Ni{sub 79.7}Fe{sub 14.0}Co{sub 2.8}Zr{sub 2.0}Cu{sub 1.5} thin film
The structure and magnetoresistance R of thin films based on Ni{sub 80}Fe{sub 20} permalloy doped with Co, Zr, and Cu have been examined by X-ray diffraction analysis and resistance measurement. The films have been obtained by ion plasma sputtering on oxidized silicon, fused quartz, and glass ceramic cold substrates. It has been shown that the structure of a film in the initial state is a mixture of solid solutions based on two phases: Ni(fcc) particles with a size of L Almost-Equal-To 8 nm and (Zr{sub 0.67}Ni{sub 0.22}O{sub 0.11}){gamma} particles with a size of L Almost-Equal-To 12 nm. The R(H) dependences on the strength and direction of the magnetic field H have been obtained at room temperature for film samples in the initial state and after isothermal annealing at 653 K for 1 h. According to R(H) dependences and X-ray diffraction analysis, films in the initial state are assumingly in a superparamagnetic state, whereas they exhibit ferromagnetic properties after isothermal annealing.
ESR and Mössbauer Spectroscopic Study of Sr-Doped Ytterbium Ferromanganites
In this paper, we have studied the crystal structure of strontium-substituted manganite and ytterbium ferromanganites Yb{sub 0.82}Sr{sub 0.18}Mn{sub 1–} {sub x}Fe{sub x}O{sub 3} (x = 0–0.2) by using X-ray diffraction analysis. Magnetic microstructure has been studied by electron paramagnetic resonance and nuclear gamma-resonance (Mössbauer) spectroscopy. We have observed phase separation in the ceramics for antiferromagnetic, superparamagnetic, and ferromagnetic phases.
Properties of MgFe{sub 2}O{sub 4} Nanoparticles Synthesized by Ultrasonic Aerosol Pyrolysis for Biomedical Applications
We present the data of studies on the structure, phase states, and magnetic properties of magnetic nanoparticles (MNPs) of magnesium ferrite spinel (MgFe{sub 2}O{sub 4}), synthesized by ultrasonic aerosols pyrolysis. Primary single-phase MNPs with an average size of 9.6, 11.5, and 14.0 nm, synthesized from precursors at concentrations of 0.06, 0.12, and 0.24 M, respectively, agglomerate into tightly aggregated spherical particles (secondary particles) with sizes of 206, 300, and 340 nm, respectively. Primary particles inside the spheres do not interact with each other and are in a superparamagnetic state. There is a layer on the surface of the particles, the magnetic structure of which differs from the structure of the inner part of the MNP; this is explained by the formation of a canted spin structure or a spin glass state in the surface layer of the MNPs. MgFe{sub 2}O{sub 4} nanospheres obtained from a precursor at a concentration of 0.06 M are most promising as valid sources of heat in magnetic hyperthermia therapy.
Obtaining Iron-Oxide Films on Sapphire Substrates
Iron-oxide films on sapphire substrates were obtained using laser radiation with 1064-nm wavelength and studied by methods of scanning electron microscopy, energy-dispersive X-ray spectroscopy, and transmission Mössbauer spectroscopy. The obtained Fe{sub 2}O{sub 3} films probably occur in a superparamagnetic state and may find application in gas sensors and various magnetic devices.
Radiative Grain Alignment in Protoplanetary Disks: Implications for Polarimetric Observations
We apply the theory of radiative torque (RAT) alignment for studying protoplanetary disks around a T-Tauri star and perform 3D radiative transfer calculations to provide the expected maps of polarized radiation to be compared with observations, such as with ALMA. We revisit the issue of grain alignment for large grains expected in the protoplanetary disks and find that mm-sized grains at the midplane do not align with the magnetic field since the Larmor precession timescale for such large grains becomes longer than the gaseous damping timescale. Hence, for these grains the RAT theory predicts that the alignment axis is determined by the grain precession with respect to the radiative flux. As a result, we expect that the polarization will be in the azimuthal direction for a face-on disk. It is also shown that if dust grains have superparamagnetic inclusions, magnetic field alignment is possible for (sub-)micron grains at the surface layer of disks, and this can be tested by mid-infrared polarimetric observations.
Nanostructured materials for selective collection of trace-level metals from aqueous systems.
Nanostructured materials for selective collection of trace-level metals from aqueous systems A critical ability for responding to situations involving environmental contaminants is the ability to quickly identify the contaminant(s) involved and the scope of the contamination. Simple field-screening methods are needed to enable on-site, information allocation and decision making. Currently, analytical technology does not exist to allow quick, accurate, and efficient analysis. Existing field-screening methods lack the selectivity and sensitivity needed to provide key information. A large leap in performance is needed and is very unlikely to be achieved with incremental improvements in procedure, instrument design, or improved electronics. A new analytical approach is required. Deficiencies in selectivity and sensitivity can be addressed with high-performance sorbent materials capable of selectively concentrating the target analytes and removing them from the sample matrix. By concentrating and removing the target analyte, these sorbent materials provide a well-defined matrix for analysis. This chapter examines the use of nanostructured materials for the selective collection of trace-level metals from aqueous systems. The focus lies on thiol-functionalized materials. Focusing on thiol surface chemistry allows comparison of mesoporous silica, activated carbon, and superparamagnetic nanoparticles. The chapter also discusses zeolites, imprinted polymer materials, and activated carbon in general. The materials reviewed here are evaluated based on capacity, selectivity, and affinity for target analytes. Research presented here shows that correctly constructed nanostructured materials are superior to conventional sorbents.
Chitosan-Gated Magnetic-Responsive Nanocarrier for Dual-Modal Optical Imaging, Switchable Drug Release, and Synergistic Therapy
In this study, we present a multifunctional yet structurally simple nanocarrier that has a high drug loading capacity, releases drug in response to onset of an AC magnetic field, and can serve as a long-term imaging contrast agent and effectively kills cancer cells by synergistic action. This nanocarrier (HMMC-NC) has a spherical shell structure with a center cavity of 80 nm in diameter. The shell is comprised of two layers: an inner layer of magnetite that exhibits superparamagnetism and an outer layer of mesoporous carbon embedded with carbon dots that exhibit photoluminescence property. Thus in addition to being a drug carrier, HMMC-NC is also a contrast agent for bioimaging. The switchable drug release is enabled by the chitosan molecules attached on the nanocarrier as the switching material which turns on or off the drug release in response to the application or withdrawal of an AC magnetic field.
Dual-Responsive Turn-On T 1 Imaging-Guided Mild Photothermia for Precise Apoptotic Cancer Therapy
Apoptosis has gained increasing attention in cancer therapy as an intrinsic signaling pathway, which leads to minimal leakage of waste products from a dying cell to neighboring normal cells. Among various stimuli to trigger apoptosis, mild hyperthermia is attractive but confronts limitations of non-specific heating and acquired resistance from elevated expression of heat shock proteins. Here, a dual-stimulation activated turn-on T 1 imaging-based nanoparticulate system (DAS) is developed for mild photothermia (≈43 °C)-mediated precise apoptotic cancer therapy. In the DAS, a superparamagnetic quencher (ferroferric oxide nanoparticles, Fe 3 O 4 NPs) and a paramagnetic enhancer (Gd-DOTA complexes) are connected via the N6-methyladenine (m 6 A)-caged, Zn 2+ -dependent DNAzyme molecular device. The substrate strand of the DNAzyme contains one segment of Gd-DOTA complex-labeled sequence and another one of HSP70 antisense oligonucleotide. When the DAS is taken up by cancer cells, overexpressed fat mass and obesity-associated protein (FTO) specifically demethylates the m 6</-sup>A group, thereby activating DNAzymes to cleave the substrate strand and simultaneously releasing Gd-DOTA complex-labeled oligonucleotides. The restored T 1 signal from the liberated Gd-DOTA complexes lights up the tumor to guide the location and time of deploying 808 nm laser irradiation. Afterward, locally generated mild photothermia works in concert with HSP70 antisense oligonucleotides to promote apoptosis of tumor cells. This highly integrated design provides an alternative strategy for mild hyperthermia-mediated precise apoptotic cancer therapy.
Multihead Attention U‐Net for Magnetic Particle Imaging–Computed Tomography Image Segmentation
Magnetic particle imaging (MPI) is an emerging noninvasive molecular imaging modality with high sensitivity and specificity, exceptional linear quantitative ability, and potential for successful applications in clinical settings. Computed tomography (CT) is typically combined with the MPI image to obtain more anatomical information. Herein, a deep learning‐based approach for MPI‐CT image segmentation is presented. The dataset utilized in training the proposed deep learning model is obtained from a transgenic mouse model of breast cancer following administration of indocyanine green (ICG)‐conjugated superparamagnetic iron oxide nanoworms (NWs‐ICG) as the tracer. The NWs‐ICG particles progressively accumulate in tumors due to the enhanced permeability and retention (EPR) effect. The proposed deep learning model exploits the advantages of the multihead attention mechanism and the U‐Net model to perform segmentation on the MPI‐CT images, showing superb results. In addition, the model is characterized with a different number of attention heads to explore the optimal number for our custom MPI‐CT dataset.
Plasmonic-magnetic bifunctional nanoparticles.
An amorphous seed-mediated strategy has been developed for the synthesis of hybrid nanoparticles that are composed of silver (yellow) and iron oxide (blue) nanodomains and exhibit unique optical properties. These properties originate from both the strong surface plasmon resonance of the silver and the strong superparamagnetic responses of the iron oxide nanodomains.
The Electrochemical Sodiation of FeSb 2 : New Insights from Operando 57 Fe Synchrotron Mössbauer and X-Ray Absorption Spectroscopy
Operando Sb K–edge X–ray absorption spectroscopy and 57 Fe Synchrotron Mössbauer Spectroscopy, used for the first time in the field of operando energy storage materials, assisted by operando magnetic measurements, were combined to clarify the role of iron and antimony in the electrochemical reaction mechanism of FeSb 2 as negative electrode material for sodium–ion batteries (SIB). Both datasets were analyzed using an innovative chemometric approach involving principal component analysis (PCA) and multivariate curve resolution – alternating least square analysis (MCR–ALS) yielding new insights on the sodiation reaction. Our findings show that the reaction of Na with FeSb 2 during discharge leads to the formation of Na 3 Sb along with superparamagnetic Fe amorphous nanoparticles which contain small amounts of Sb dissolved in their lattice. During the following desodiation, the pristine material FeSb 2 is not recovered while iron nanoparticles grow in size, and continue growing also along the following discharge. Here, even though such iron nanoparticles remain electrochemically inactive, they play a key role in the reduction and stabilization of the polarization as well as in the reversibility of the electrochemical sodiation of antimony.
Fe 3 O 4 Nanoparticles Anchored on Carbon Serve the Dual Role of Catalyst and Magnetically Recoverable Entity in the Aerobic Oxidation of Alcohols
Carbon supported γ-Fe2O3 nanoparticle (γ-Fe2O3/C) possessing both superparamagnetism and activating molecular oxygen properties were prepared by an ammonia-assisted precipitation method. It could catalyze the selective oxidation of various benzyl alcohols with air as oxidant source, and could be easily recycled with an external magnet separation. The correlation between the intrinsic properties of γ-Fe2O3 nanoparticles and the catalytic performance was investigated with a series of characterizations. It shows that the oxidation state of γ-Fe2O3 nanoparticles were facile to be changed, which should be related to its inverse spinel type crystal structure with vacant cation sites. These γ-Fe2O3 nanoparticles should be the active sites and responsible for the high activity of γ-Fe2O3/C in the air oxidation of alcohols. The formation of γ-Fe2O3 nanoparticle was controlled by precipitation agent and carbon support. Using ammonia ethanol solution as precipitation agent, the hydrolysis rate of iron species could be decreased. The surface functional groups of carbon support could act as chelating sites for iron species, controlling the nucleation and growth of the γ-Fe2O3 nanoparticles in the preparation process. Dr. Xiang Wang gratefully acknowledges the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division for the support of this work.
Dilute Magnetic Semiconductors from Electrodeposited ZnO Nanowires
We present experimental results on the magnetic properties of doped ZnO nanowires grown at 80 8C in electrodeposition. We show that impurities such as Al, Mn, Co, and Cu can be incorporated in the nanowires by adding the corresponding metal salts to the electrolyte solution. At concentration levels of a few atomic percent we find the impurity concentration in the solid to be approximately proportional to the precursor concentration in solution. ZnO nanowrires doped with Cu, Co, and Mn show superparamagnetic response at room temperature, while undoped and Al-doped wires show no discernible magnetic response. The results indicate that with Cu, Mn, and Co doping dilute magnetic semiconductors can be prepared.
Magnetic Particle Imaging Guided Real-Time Percutaneous Transluminal Angioplasty in a Phantom Model
PurposeTo investigate the potential of real-time magnetic particle imaging (MPI) to guide percutaneous transluminal angioplasty (PTA) of vascular stenoses in a phantom model.Materials and MethodsExperiments were conducted on a custom-built MPI scanner. Vascular stenosis phantoms consisted of polyvinyl chloride tubes (inner diameter 8 mm) prepared with a centrally aligned cable tie to form ~ 50% stenoses. MPI angiography for visualization of stenoses was performed using the superparamagnetic iron oxide nanoparticle-based contrast agent Ferucarbotran (10 mmol (Fe)/l). Balloon catheters and guidewires for PTA were visualized using custom-made lacquer markers based on Ferucarbotran. Stenosis dilation (n = 3) was performed by manually inflating the PTA balloon with diluted Ferucarbotran. An online reconstruction framework was implemented for real-time imaging with very short latency time.ResultsVisualization of stenosis phantoms and guidance of interventional instruments in real-time (4 frames/s, ~ 100 ms latency time) was possible using an online reconstruction algorithm. Labeling of guidewires and balloon catheters allowed for precise visualization of instrument positions.ConclusionReal-time MPI-guided PTA in a phantom model is feasible.
Magnetic Behavior of Iron-Rich Permalloy Nanoparticles
Iron-rich permalloy Fe{sub x}Ni{sub 1−x} nanoparticles (NPs) were fabricated using a low-temperature wet chemistry method involving the hydrothermal growth of the NPs. Three Fe–Ni NPs (Fe{sub 0.5}Ni{sub 0.5}, Fe{sub 0.625}Ni{sub 0.375}, and Fe{sub 0.83}Ni{sub 0.17}) were fabricated and studied by X-ray diffraction (XRD), scanning electron microscopy (SEM), and vibrating sample magnetometer (VSM). After the initial formations, the three Fe–Ni NPs were annealed at 200, 400, and 600 °C; the XRD showed that all three FeNi NPs had a bcc structure (not the fcc structure of the standard Fe{sub 20}Ni{sub 80} permalloy). The SEM images showed that the NPs had spherical shapes. The VSM measurements showed that none of the Fe–Ni nanoparticles were superparamagnets but were ferromagnets. The heat treatments cause the work needed to the flip the spin (coercivity (H{sub c})) to increase and the values of the saturation magnetizations to fluctuate.