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At least 55 records · Page 3

DNA-caged nanoparticles via electrostatic self-assembly

DNA-modified nanoparticles enable DNA sensing and therapeutics in nanomedicine and are also crucial for nanoparticle self-assembly with DNA-based materials. However, methods to conjugate DNA to nanoparticle surfaces are limited, inefficient, and lack control. Inspired by DNA tile nanotechnology, we demonstrate a new approach to nanoparticle modification based on electrostatic attraction between negatively charged DNA tiles and positively charged nanoparticles. This approach does not disrupt nanoparticle surfaces and leverages the programmability of DNA nanotechnology to control DNA presentation. We demonstrated this approach using a variety of nanoparticles, including polymeric micelles, polystyrene beads, gold nanoparticles, and superparamagnetic iron oxide nanoparticles with sizes ranging from 5–20 nm in diameter. DNA cage formation was confirmed through transmission electron microscopy (TEM), neutralization of zeta potential, and a series of fluorescence experiments. DNA cages present “handle” sequences that can be used for reversible target attachment or self-assembly. Handle functionality was verified in solution, at the solid–liquid interface, and inside fixed cells, corresponding to applications in biosensing, DNA microarrays, and erasable immunocytochemistry. Finally, these experiments demonstrate the versatility of the electrostatic DNA caging approach and provide a new pathway to nanoparticle modification with DNA that will empower further applications of these materials in medicine and materials science.

60 APPLIED LIFE SCIENCES↗

Resilience of the Aurivillius structure upon La and Cr doping in a Bi 5 Ti 3 FeO 15 multiferroic

Here, combining the experimental techniques of high-resolution X-ray diffraction, magnetometry, specific heat measurement, and X-ray photoelectron, Raman and dielectric spectroscopy techniques, we have studied the influence of La and Cr doping on the crystal structure and magnetism of the room temperature Aurivillius multiferroic Bi 5 Ti 3 FeO 15 by investigating the physical properties of (Bi 4 La)Ti 3 FeO 15 and Bi 5 Ti 3 (Fe 0.5 Cr 0.5 )O 15 . The parent (Bi 5 Ti 3 FeO 15 ) and the doped ((Bi 4 La)Ti 3 FeO 15 and Bi 5 Ti 3 (Fe 0.5 Cr 0.5 )O 15 ) compounds crystallize in the A2 1 am space group, which is confirmed through our analysis of high-resolution synchrotron X-ray diffraction data obtained on phase-pure polycrystalline powders. We determined the oxidation states of the metal atoms in the studied compounds as Fe 3+ , Ti 4+ , Cr 3+ , and La 3+ through the analysis of X-ray photoelectron spectroscopy data. The magnetic susceptibilities of the three compounds are marked by the absence of a long-range ordered ground state, but dominated by superparamagnetic clusters with dominant antiferromagnetic interactions. This signature of short-range magnetism is also seen in specific heat as a low temperature enhancement which is suppressed upon the application of external magnetic fields up to 8 T. Our dielectric spectroscopy experiments showed that the three studied compounds display similar features in the dielectric constant measured as a function of frequency. However, upon doping La at the Bi site, the width of the ferroelectric hysteresis loop increases for (Bi 4 La)Ti 3 FeO 15 compared to that of the parent compound Bi 5 Ti 3 FeO 15 , and with Cr doping, Bi 5 Ti 3 (Fe 0.5 Cr 0.5 )O 15 becomes a leaky dielectric. The resilience of the Aurivillius crystal structure towards doping of La at the Bi site and Cr at the Fe site is clearly seen in the bulk properties of magnetic susceptibility, specific heat and the average crystal structure. The relevance of changes in the local structure is evident from our Raman spectroscopy and X-ray pair distribution function studies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Spin dynamics and relaxation in 7.6 nm thin film of La 0.7 Sr 0.3 MnO 3 /SrTiO 3 : ac magnetic susceptibility and magnetic viscosity investigations

Analysis of the results from our investigations of the temperature dependence of ac susceptibilities (χ' and χ'') and magnetic viscosity in a 7.6 nm thin film of La 0.7 Sr 0.3 MnO 3 grown on SrTiO 3 (001) substrate is presented. The Curie temperature (T C ) of this film is magnetic field (H) dependent, varying as [T C (H) - T C (0)] ~ H n with T C (0) = 270 K and n = 0.15. Temperature dependence of χ' and χ'' measured at ac frequencies f m in the range of 0.1–10 kHz shows a broad peak near 230 K associated with the blocking temperature (T B ) of spin clusters present in the 1.4 nm surface layer and a frequency dependent peak near 270 K associated with T C . The mean relaxation time τ determined from the Cole–Cole analysis of the temperature dependent χ' and χ'' is shown to fit the Vogel–Fulcher law: τ = τ 0 exp[ΔE/k B (T - T 0 )] with T 0 = 245 K, ΔE/k B = 270 K = T C and τ 0 = 1.2 x 10 -9 s. Magnetic viscosity S (measured in H = 0 for a sample cooled in H = 50 Oe) determined from the fit to the magnetization: M (t)= M (0) – S ln t, with time t up to 2 h, shows a peak at 230 K above which M (2 h) switches to negative values for temperatures up to T C (0). It is argued that this negative magnetization results from an interaction between the superparamagnetic spin clusters and the ferromagnetic phase, both being present in the temperature range of T B < T < T C .

36 MATERIALS SCIENCE↗

Coexistence of soft and hard magnetic phases in single layer amorphous Tb–Co thin films

Amorphous, ferrimagnetic Tb-Co thin films prepared with a thin Ta underlayer and either a Ta or a Pt overlayer show evidence of both soft and hard magnetic phases. At room temperature, the films exhibit conventional ferromagnetism, but low temperature magnetometry measurements reveal the decoupling of the two magnetic phases with decreasing temperature due to increased anisotropy energy of the hard layer at lower temperatures. Decreasing the film thickness to 2 nm, slightly above the superparamagnetic limit found at 1 nm, a soft, low-density phase was isolated and found to be present in all the films as confirmed with x-ray reflectivity and Rutherford backscattering spectrometry measurements. For greater thicknesses, the bottom layer retains its soft magnetic nature, while the remainder of the film is denser and has strong perpendicular magnetic anisotropy, leading to the exchange-spring behavior when the anisotropy becomes large, either at low temperatures or via a Pt overlayer that adds a strong interfacial anisotropy to the layer. Micromagnetic simulations of a soft/hard bilayer model with the experimentally determined anisotropy and magnetization parameters into a soft/hard bilayer model reproduced the experimental hysteretic behavior very well. These findings demonstrate how the magnetic state and the response of a-Tb-Co films to external fields can be controlled, providing a high degree of tunability that is promising for high-performance nanoscale devices.

36 MATERIALS SCIENCE↗

An alternative ground state of MnBi 2 Te 4 obtained by magnetic annealing

Magnetic topological insulators are extremely interesting because they combine the unique properties of topological insulators with magnetism. While as-grown MnBi 2 Te 4 single crystals exhibit an A-type antiferromagnetic (AFM) ordering at T N ≈ 24 K, annealed MnBi 2 Te 4 under 10 T leads to the change of the magnetic properties from AFM to superparamagnetic behavior with the trend of the magnetization saturation at 2 K. Correspondingly, the magnetotransport properties change as well, revealing large positive magnetoresistance with the linear field dependence at low temperatures. Through the first-principles calculations, we provide insight into the experimental results. Our investigation demonstrates that magnetic annealing is a powerful approach for manipulating material properties due to the nearly degenerate ground states in MnBi 2 Te 4 .

Electronic transport↗

Significance of the structural configuration of B2 disorder in Co and Ti based Heusler alloys

We investigate here structural (at local and global levels) and transport properties for 𝑋 2 ⁢MnAl (𝑋= Co and Ti). Additionally, the magnetic properties were also studied for Ti 2 ⁢MnAl. Our x-ray diffraction results show that both the compounds stabilize in B2 disordered phase with cubic structure of 𝑃⁢𝑚⁢$\overline{3}$⁢𝑚 space group. Further, the structural configuration of the above disordered phase for both the compounds was identified using combined studies of x-ray absorption spectroscopy and multiple scattering calculations at the transition metal 𝐾 edges. Upon such identification, in the case of Co 2 ⁢Mn 1−𝑦⁢ Cr 𝑦 ⁢Al (𝑦= 0, 0.05, 0.1, 0.2) with change in 𝑦, we are able to establish a better connection quantitatively between the inverse of Mn-Co bonds and peak in the temperature-dependent resistivity. This highlights the crucial importance of a detailed understanding of the nature of B2 disorder. In the case of 𝑦=0, in the temperature range of study, the resistivity is driven by the functional form associated with (a) three-dimensional enhanced electron-electron Coulomb interaction scattering mechanism and (b) an unconventional one-magnon process. For Ti 2 ⁢MnAl, the transport shows metallic glasslike behavior at high temperature, while at low temperature it follows both the Cote-Meisel's model and quantum correction model. In this compound, the magnetic studies suggest the formation of superparamagnetic clusters in the paramagnetic matrix at low temperatures. Our density functional theory results are in line with the transport and magnetic properties. In literature, the spin polarization percentage (𝑃) for 𝑋= Co in B2 disordered phase is 76%. However, the present results emphasize the fact that in B2 disordered phase, the value of 𝑃 can range from 90% to 71% depending on the structural configuration introduced by swapping of the atomic positions of Mn and Al. For the compound under study, the value of percentage spin polarization obtained ranges between 82% to 85%. In addition, we also identify the origin of the difference in the shape of the Mn 3⁢𝑑 density of states for both the alloys. In conclusion, our results for 𝑋= Co alloy highlights the importance of identifying the specific structural configuration associated with a particular disorder category especially in the estimation of 𝑇 𝑐 and 𝑃 and for 𝑋= Ti, the physical properties can be tuned by varying the position of 𝐸 𝐹 and thereby its utilization in device applications.

36 MATERIALS SCIENCE↗

Thermally superactive artificial kagome spin ice structures obtained with the interfacial Dzyaloshinskii-Moriya interaction

Artificial kagome spin ice exhibits exotic magnetic correlations driven by a combination of geometric frustration and dipolar interactions that, at low-enough temperature, can result in ordered phases. This order, whether it is the ground state of several kagome rings, or the theoretically predicted long-range order of an extended array, has yet to be experimentally observed. By introducing an interfacial Dzyaloshinskii-Moriya interaction, we are able to reduce the blocking temperature of the individual nanomagnets, allowing a system of 30 kagome nanomagnets to explore its vast manifold of microstates and find its ground state. Furthermore, the extracted magnetic correlations in an extended artificial kagome spin ice are found to exhibit quantitative signatures of long-range charge order, providing evidence of the theoretically predicted continuous phase transition to the charge-ordered state. The significant lowering of the blocking temperature in nanomagnets is important for the exploitation of superparamagnetism in artificial spin systems and devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Lattice symmetry breaking transition and critical size limit for ferroic orders in nanophase BiFeO3

Finite size effects on the ferroic orders in BiFeO 3 are studied by atomic pair distribution function analysis and magnetic measurements. While bulk rhombohedral BiFeO 3 exhibits ferroelectricity and antiferromagnetism with a cycloidal magnetic moment arrangement leading to zero magnetization and weak magnetoelectric coupling, BiFeO 3 nanoparticles with a size smaller than the spin cycloid period of 62 nm preserve their polar rhombohedral structure and develop ferromagnetism, thus exhibiting coexisting polarization and nonzero magnetization that enhances the magnetoelectric coupling. When the nanoparticles become smaller than 17 nm, however, their crystal lattice expands and becomes nonpolar cubic. They also become superparamagnetic and thus simultaneously cease exhibiting both ferroelectricity and ferromagnetism. Our findings shed light on the interaction between the lattice structure and ferroic orders in nanophase perovskites and also provide a rare example of a lattice symmetry breaking phase transition that determines their critical size.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Structure and magnetism in epitaxial Fe 1 + x VSb nanocomposite films

The combination of ferromagnetism and semiconducting behavior offers an avenue for realizing novel spintronics and spin-enhanced thermoelectrics. Here we demonstrate the synthesis of doped and nanocomposite half-Heusler Fe 1+x VSb films by molecular beam epitaxy. For dilute excess Fe (x < 0.1), we observe a decrease in the Hall electron concentration and no secondary phases in x-ray diffraction. Magnetotransport measurements suggest weak ferromagnetism that onsets at a temperature of T c ≈ 5 K. For higher Fe content (x > 0.1), ferromagnetic Fe nanostructures precipitate from the semiconducting FeVSb matrix. The Fe/FeVSb interfaces are epitaxial, as observed by transmission electron microscopy and x-ray diffraction. Further, magnetotransport measurements suggest proximity-induced magnetism in the FeVSb from the Fe/FeVSb interfaces, or superparamagnetically coupled Fe-rich clusters, at an onset temperature of T c ≈ 20 K.

36 MATERIALS SCIENCE↗

Nonequilibrium sub-10 nm spin-wave soliton formation in FePt nanoparticles

Magnetic nanoparticles such as FePt in the L1 0 phase are the bedrock of our current data storage technology. As the grains become smaller to keep up with technological demands, the superparamagnetic limit calls for materials with higher magnetocrystalline anisotropy. This, in turn, reduces the magnetic exchange length to just a few nanometers, enabling magnetic structures to be induced within the nanoparticles. Here, we describe the existence of spin-wave solitons, dynamic localized bound states of spin-wave excitations, in FePt nanoparticles. We show with time-resolved x-ray diffraction and micromagnetic modeling that spin-wave solitons of sub–10 nm sizes form out of the demagnetized state following femtosecond laser excitation. The measured soliton spin precession frequency of 0.1 THz positions this system as a platform to develop novel miniature devices.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Probing T Cell 3D Mechanosensing With Magnetically-Actuated Structures

The ability of cells to recognize and respond to the mechanical properties of their environment is of increasing importance in T cell physiology. However, initial studies in this direction focused on planar hydrogel and elastomer surfaces, presenting several challenges in interpretation including difficulties in separating mechanical stiffness from changes in chemistry needed to modulate this property. We introduce here the use of magnetic fields to change the structural rigidity of microscale elastomer pillars loaded with superparamagnetic nanoparticles, independent of substrate chemistry. This magnetic modulation of rigidity, embodied as the pillar spring constant, changed the interaction of mouse naïve CD4 + T cells from a contractile morphology to one involving deep embedding into the array. Furthermore, increasing spring constant was associated with higher IL-2 secretion, showing a functional impact on mechanosensing. The system introduced here thus separates local substrate stiffness and long-range structural rigidity, revealing new facets of T cell interaction with their environment.

60 APPLIED LIFE SCIENCES↗

Signal Differentiation of Moving Magnetic Nanoparticles for Enhanced Biodetection and Diagnostics

Magnetic nanoparticles are extensively utilized as markers/signal labelling in various biomedical applications. Detecting and distinguishing magnetic signals from similarly sized moving magnetic nanoparticles in microfluidic systems is crucial yet challenging for biosensing. In this study, we have developed an original method to detect and differentiate magnetic signals from moving superparamagnetic (SPM) and ferrimagnetic (FM) nanoparticles of comparable sizes. Our approach utilizes a highly sensitive magnetic-coil-based sensor that harnesses the combined effects of giant magnetoimpedance (GMI) and an LC-resonance circuit, offering performance superior to that of conventional GMI sensors. Iron oxide nanoparticles, which have similar particle sizes but differing coercivities (zero for SPM and non-zero for FM) or similar zero coercivities but differing particle sizes, flow through the magnetic coil at controlled velocities. Their distinct effects are analyzed through changes in the complex impedance of the sensing system. Our findings provide a unique pathway for utilizing SPM and FM nanoparticles as innovative magnetic markers to identify specific biological entities, thereby expanding their potential applications.

Hwang, Kee Young↗

Magnetic coercivity and ferromagnetic species in lunar materials

Lunar samples have reduced coercive force, high values of R sub H (ratio of remanent coercive force to coercive force), and constriction in their magnetic hysteresis loops due to the presence of superparamagnetic and multidomain iron grains. The high R sub H values are also attributable to the magnetic shape effects of the iron grains. Spheres, cubes, and needles, as well as more irregular metal grains were observed. The coercive force values are quite meaningless unless the size and shape distributions are determined. The R sub H and the ratio of saturation remanence to saturation magnetization values can be considered characteristic of the size and shape modes of the ferromagnetic grains in a natural sample, and a classification of natural materials based on their hysteresis characteristics is presented with special reference to lunar samples.

Wasilewski, P.↗

Amorphous magnetism in fcc Vicalloy 2

The results of magnetization and Mossbauer experiments are reported which give evidence for superparamagnetism in the quenched face centered cubic (gamma) phase of the ternary system Fe(0.34)C(0.52)V(0.14) (Vicalloy 2). while the magnetization data agree with the limited data of Nesbitt et al., this more complete study shows clearly that this alloy does not acquire long-range ferromagnetic order, nor does it indicate either antiferromagnetic long-range ordering or mictomagnetic behavior, down to 4.2 K. The data can best be described as resulting from ferromagnetic clusters in a weakly magnetic lattice. The Mossbauer data show a slightly broadened single line spectrum of 300 K which broadens with decreasing temperature without development of resolvable hyperfine splitting down to 4.2 K. The broadening is attributed to relaxation effects associated with magnetic cluster coalescence.

Cusick, J. P.↗

Particle shape and magnetization of chondrite meteorites, lunar samples, and impactites

Extra terrestrial materials, certain materials which have their origin at the earth's surface due to meteoritic impact, or under highly reducing conditions, such as in the case of basaltic flows in contact with coal beds or serpentenites, all contain Fe and FeNi phases with high magnetization values and spherical shape. Normally, the demagnetizing field (H sub D = NI sub S: where N is the demagnetizing factor and I is the saturation magnetization) is corrected for. In disperse systems, such as most natural materials, the particle shape effects are analyzed in terms of the saturation fields, Hs = H sub D = NI sub S and the magnetization differences (Delta I sub S). Discrete size modes of superparamagnetic (SP), multidomain (MD), and single domain (SD) particles result in reduced coercive force (Hc), increase in the value R sub H (ratio of remanent coercive force, H sub R, to H sub C), and decrease in the value R sub I (ratio of remanent magnetization, I sub R, to saturation magnetization, T sub S). The main distinctions between the various natural materials can be made by this approach. Hysteresis loops for terrestrial basalts, Fe and Ni rods and spheres, chondrite meteorites, lunar samples, impactites, and chondritic fusion crust are presented.

Wasilewski, P.↗