FePt nanoparticles have great application potential in advanced magnetic materials such as ultrahigh-density recording media and high-performance permanent magnets. [1][2][3] The key for applications is the very high uniaxial magnetocrystalline anisotropy of the L1 0 -FePt phase, which is based on crystalline ordering of the face-centered tetragonal (fct) structure, described by the chemical-ordering parameter S.[4] Higher chemical ordering results in higher magnetocrystalline anisotropy. Unfortunately, as-synthesized FePt nanoparticles take a disordered face-centered cubic (fcc) structure that has low magnetocrystalline anisotropy. Heat-treatment is necessary to convert the fcc structure to the ordered fct structure. Several previous theoretical and experimental investigations have been reported on the size-dependent chemical ordering of FePt nanoparticles. [5][6][7][8][9] It has been observed that the degree of ordering decreases with decreasing particle size of the sputtered FePt nanoparticles. [5,6] Theoretical simulation predicted that the ordering would not take place when the particle size is below a critical value. [8,9] However, there have not been systematic experimental studies on quantitative size dependence of chemical ordering of FePt nanoparticles due to the lack of monodisperse L1 0 -FePt nanoparticles with controllable sizes.There are also few studies reported to date on the quantitative particle size dependence of magnetic properties, including the Curie temperature, coercivity, and magnetization of the L1 0 -FePt phase, although it has been well accepted that there is a size effect on the ferromagnetism of any low-dimensional magnets. [10,11] Additionally, the magnetic properties of FePt ferromagnets, as observed in thin-film samples, [4,12] are affected by the degree of chemical ordering, which is in turn size dependent. It is therefore highly desirable to understand the size and chemical-ordering effects, and their influence on the magnetic properties of the nanoparticles. A major hurdle in obtaining the particle size dependence of structural and magnetic properties of the L1 0 phase is particle sintering during heat-treatments that convert the fcc phase to the fct phase. [13,14] This long-pending problem has been solved recently by adopting the salt-matrix annealing technique. [15,16] With this technique, particle aggregation during the phase transformation has been avoided so that the true size-dependent properties of the fct phase can be measured. In this paper, we report results on quantitative particle size dependence of the chemical-ordering parameter S and selected magnetic properties, including the Curie temperature, T c , magnetization, M s , and coercivity, H c , with the particle size varying from 2 to 15 nm. Figure 1 shows the transmission electron microscopy (TEM) images of the FePt nanoparticles with different sizes before and after annealing in a salt matrix at 973 K for 4 h. The images, from left to right, show nanoparticles with nominal diameters of 2, 4, 6, 8, and 15 nm, res...
Monodisperse face-centred tetragonal (fct) FePt nanoparticles with high magnetic anisotropy and, therefore, high coercivity have been prepared via a new heat treatment route. The as-synthesized face-centred cubic FePt nanoparticles were mixed with salt powders and annealed at 700˚C. The salts were then removed from the particles by washing the samples in water. Monodisperse fct FePt particles were recovered with the particle size and shape being retained. Coercivity of the isolated particles up to 30 kOe at room temperature has been obtained.
Morphological control of FePt nanoparticles has been systematically studied. By varying synthetic parameters including precursors, solvents, amount of surfactants, and heating rate of the solution, the particle size from 2 to 9 nm can be tuned with 1 nm accuracy. While most particles are spherical in shape, cubic particles can be obtained when particles are greater than 7 nm. Rod-shape nanoparticles have also been obtained. The as-synthesized nanoparticles are found to be superparamagnetic at room temperature and their blocking temperature is size dependent that increases with particle size. After annealing in a reducing atmosphere, the nanoparticles form hard magnetic films with ordered fct structure and high coercivity up to 2.7 T.
A 27 amino acid collagen-based peptide (Hbyp3) was designed to radially display nine hydrophobic bipyridine moieties from a triple helical scaffold. Self-assembly of such functionalized triple helices led to the formation of micrometer-scaled disks with a curved morphology, presumably mediated by aromatic interactions, with a height that is in the range of the length of the triple helical peptide. Higher order assembly of these curved disks into micrometer-sized hollow spheres was accomplished through metal-ligand interactions between bipyridine groups of the disks and metal ions such as Fe(II), Co(II), Zn(II) and Cu(II). The thickness of the shell of these hollow spheres corresponds well with the thickness of the collagen peptide-based triple helix and the corresponding self-assembled disks. Addition of a metal ion chelator was found to reverse the assembly of the hollow spheres back to the curved disk structures. These data support the formation of the hollow spheres from the self-assembled disks of Hbyp3 upon addition of metal ions.
Magnetic nanostructures (MNS) have emerged as promising functional probes for simultaneous diagnostics and therapeutics (theranostic) applications due to their ability to enhance localized contrast in magnetic resonance imaging (MRI) and heat under external radio frequency (RF) field, respectively. We show that the "theranostic" potential of the MNS can be significantly enhanced by tuning their core composition and architecture of surface coating. Metal ferrite (e.g., MFe2O4) nanoparticles of ∼8 nm size and nitrodopamine conjugated polyethylene glycol (NDOPA-PEG) were used as the core and surface coating of the MNS, respectively. The composition was controlled by tuning the stoichiometry of MFe2O4 nanoparticles (M = Fe, Mn, Zn, ZnxMn1-x) while the architecture of surface coating was tuned by changing the molecular weight of PEG, such that larger weight is expected to result in longer length extended away from the MNS surface. Our results suggest that both core as well as surface coating are important factors to take into consideration during the design of MNS as theranostic agents which is illustrated by relaxivity and thermal activation plots of MNS with different core composition and surface coating thickness. After optimization of these parameters, the r2 relaxivity and specific absorption rate (SAR) up to 552 mM(-1) s(-1) and 385 W/g were obtained, respectively, which are among the highest values reported for MNS with core magnetic nanoparticles of size below 10 nm. In addition, NDOPA-PEG coated MFe2O4 nanostructures showed enhanced biocompatibility (up to [Fe] = 200 μg/mL) and reduced nonspecific uptake in macrophage cells in comparison to other well established FDA approved Fe based MR contrast agents.
Bimagnetic FePt/ Fe 3 O 4 nanoparticles with core/shell or heterodimer structure have been prepared using a sequential synthetic method. The dimension of both FePt and Fe 3 O 4 was tuned by varying the synthesis parameters. The as-synthesized bimagnetic nanoparticles were superparamagnetic at room temperature. After being annealed in a reducing atmosphere, the FePt/ Fe 3 O 4 bimagnetic nanoparticles were converted to a hard magnetic nanocomposite with enhanced energy products due to the exchange coupling between the hard and soft magnetic phases. It was found that the exchange coupling in nanocomposites made from the core/shell nanoparticles is stronger than that from the heterodimer nanoparticles. By tuning the dimensions of the FePt and Fe 3 O 4 phases, the energy product up to 17.8 MGOe was achieved in the annealed nanocomposites, which is 36% higher than the isotropic single-phase FePt counterpart.
To transfer face-centered-cubic ͑fcc͒ FePt nanoparticles to the face-centered-tetragonal ͑fct͒ phase with high magnetic anisotropy, heat treatments are necessary. The heat treatments lead to agglomeration and sintering of the nanoparticles. To prevent the particles from sintering, salts as the separating media ͑matrix͒ have been used for annealing the nanoparticles in our experiments. The fcc nanoparticles produced by chemical synthesis were mixed with NaCl powders. The mixture was then annealed in forming gas ͑93% H 2 +7%Ar͒ in different conditions to complete the fcc to fct phase transition. After the annealing, the salt was washed out by water and monodisperse fct FePt nanoparticles were obtained. Detailed studies on the effect of the NaCl-to-FePt weight ratios ͑from 1:1 to 400:1͒ have been performed. It was found that a suitable NaCl-to-FePt ratio is the key to obtain monodisperse fct FePt nanoparticles. A higher NaCl-to-FePt ratio is needed for larger particles when the annealing conditions are the same. Increased annealing temperature and time should be accompanied by a higher NaCl-to-FePt ratio. Magnetic measurements show very high coercivity ͑up to 30 kOe͒ of the monodispersed fct nanoparticles by the salt-matrix annealing. 1 The chemically synthesized FePt nanoparticles, however, are of face-centered-cubic ͑fcc͒ phase without magnetic anisotropy. To transfer FePt nanoparticles from fcc phase to face-centered-tetragonal ͑fct͒ phase, heat treatments above 600°C are necessary, which undesirably lead to sintering of these nanoparticles.Since 2000, great efforts have been made to produce monodisperse fct FePt nanoparticles 2-8 driven by potential applications of the magnetically anisotropic nanoparticles in high-density recording media and high-performance nanocomposite magnets. Recently, we obtained monodisperse fct FePt nanoparticles with retained size and shape by using salts as the annealing separating media. 9 The salts can be completely removed after the annealing just by washing the samples in water. High coercivity up to 30 kOe of the fct particles has been obtained. In this paper we report detailed results in controlling the particle morphology and properties by adjusting the salt-to-FePt particle ratio. EXPERIMENTThe fcc FePt nanoparticles with size of 4, 8, and 15 nm were synthesized by chemical solution methods.1,10-13 Sodium chloride ͑NaCl͒ was selected as a separating media in this investigation due to its chemical stability and high solubility in water. NaCl was first ball milled for 24 h to reduce the particle size. The ball-milled NaCl powder was then dispersed in hexane and mixed with hexane dispersion of assynthesized fcc FePt nanoparticles. The mixture was stirred until all the solvent evaporates. Then the mixture was annealed in forming gas ͑93% H 2 +7%Ar͒ in different conditions to complete the fcc to fct transition. The annealed powders were washed in de-ionized water and centrifuged for several times to remove all the NaCl.9 Different NaCl-toFePt weight ratios from 1:1 to 400:1 were t...
Flavins feature multiple attributes that explain their widespread occurrence in nature, including photostability, reversible electrochemistry, and especially the tunability of their optical, electronic, and redox properties by supramolecular interactions and modification of their chemical structure. Flavins are important redox cofactors for enzymatic catalysis and are central to a wide variety of processes, including biosynthesis, electron transport, photosynthesis, and DNA repair. The wide range of processes catalyzed by flavins makes them promising leads for synthetic catalysts. Their properties are also relevant to organic electronic and optoelectronic devices, where they have the potential to serve as photoactive electron carriers, a very uncommon property in current photovoltaic systems. In flavoenzymes, the flavin cofactor binds to the active site of the apoenzyme through noncovalent interactions. These interactions regulate cofactor recognition and tune the redox behavior of the flavin cofactor. In this Account, we describe the creation of host-guest systems based on small molecule, polymer, and nanoparticle scaffolds that explore the role of aromatic stacking on the redox properties of the flavin and provide insight into flavoenzyme function. We also describe the creation of synthetic flavin-based interlocked structures featuring aromatic stacking interactions, along with the use of aromatic stacking to direct self-assembly of flavin-based materials. The interplay between redox events and aromatic stacking interactions seen in these synthetic models is important for fundamental understanding of biological systems including the flavoenzymes. The precise control of aromatic interactions and binding of flavins not only underpins their biological activity but gives them the potential to be developed into novel organic optoelectronic materials based on tuned synthetic flavin-receptor assemblies. In a broader context, the redox properties of the flavin provide a very concise tool for looking at the role of electronics in aromatic stacking, an issue of general importance in biological and supramolecular chemistry.
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