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Growth and characterization of ferromagnetic Ga2O3:(Cr, Mn)

Sapkota, Keshab R.; Wang, George T.; Addamane, Sadhvikas J.; Lu, Tzu M.; Zhao, Hongping; Monson, Todd; Pearce, Charles J.; Sharps, Paul

The goal of this Exploratory Express project was to explore the possibility of tunable ferromagnetism in Mn or Cr incorporated epitaxial Ga2O3 films. Tunability of magnetic properties can enable novel applications in spintronics, quantum computing, and magnetism-based logics by allowing control of magnetism down to the nanoscale. Carriers (electrons or holes) mediated ferromagnetic ordering in semiconductor can lead to tunable ferromagnetism by leveraging the tunability of carrier density with doping level, gate electric field, or optical pumping of the carriers. The magnetic ions (Cr or Mn) in Ga2O3 act as localized spin centers which can potentially be magnetically coupled through conduction electrons to enable ferromagnetic ordering. Here we investigated tunable ferromagnetism in beta Ga2O3 semiconductor host with various n-doping levels by incorporating 2.4 atomic percent Mn or Cr. The R&D approach involved growth of epitaxial Ga2O3 film on sapphire or Ga2O3 substrate, implantation of Mn or Cr ions, annealing of the samples post implantation, and magnetic measurements. We studied magnetic behavior of Mn:Ga2O3 as a function of different n-doping levels and various annealing temperatures. The vibrating sample magnetometry (VSM) measurement exhibited strong ferromagnetic signals from the annealed Mn:Ga2O3 sample with n-doping level of 5E19 cm-3. This ferromagnetic behavior disappears from Mn:Ga2O3 when the n-doping level is reduced to 5E16 cm-3. Although these results are to be further verified by other measurement schemes due to the observation of background ferromagnetism from the growth substrate, these results indicate the possibility of tunable ferromagnetism in Mn:Ga2O3 mediated by conduction electrons.

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Negligible magnetic losses at low temperatures in liquid phase epitaxy grown Y3Fe5O12 films

Physical Review Materials

Will-Cole, A.R.; Hart, James L.; Lauter, Valeria; Grutter, Alexander; Dubs, Carsten; Lindner, Morris; Reimann, Timmy; Pearce, Charles J.; Monson, Todd; Cha, Judy J.; Heiman, Don; Sun, Nian X.

Yttrium iron garnet (Y3Fe5O12; YIG) has a unique combination of low magnetic damping, high spin-wave conductivity, and insulating properties that make it a highly attractive material for a variety of applications in the fields of magnetics and spintronics. While the room-temperature magnetization dynamics of YIG have been extensively studied, there are limited reports correlating the low-temperature magnetization dynamics to the material structure or growth method. Here, in this study, we investigate liquid phase epitaxy grown YIG films and their magnetization dynamics at temperatures down to 10 K. We show there is a negligible increase in the ferromagnetic resonance linewidth down to 10 K, which is unique when compared with YIG films grown by other deposition methods. From the broadband ferromagnetic resonance measurements, polarized neutron reflectivity, and scanning transmission electron microscopy, we conclude that these liquid phase epitaxy grown films have negligible rare-earth impurities present, specifically the suppression of Gd diffusion from the Gd3Ga5O12 (GGG) substrate into the Y3Fe5O12 film, and therefore negligible magnetic losses attributed to the slow-relaxation mechanism. Overall, liquid phase epitaxy YIG films have a YIG/GGG interface that is five times sharper and have ten times lower ferromagnetic resonance linewidths below 50 K than comparable YIG films by other deposition methods. Thus, liquid phase epitaxy grown YIG films are ideal for low-temperature experiments/applications that require low magnetic losses, such as quantum transduction and manipulation via magnon coupling.

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Fabrication and characterization of net-shaped iron nitride-amine-epoxy soft magnetic composites

Frontiers in Materials

Hoyt, Melinda R.; Falcon, Gillian I.; Pearce, Charles J.; Stevens, Tyler E.; Johnson, Emily M.; Szenderski, Thomas M.; Sorenson, Nathan R.; Fultz-Waters, Sydney F.; Rodriguez, Mark A.; Whalen, Lisa J.; Monson, Todd; Delaney, Robert E.

Soft magnetic composites (SMCs) offer a promising alternative to electrical steels and soft ferrites in high performance motors and power electronics. They are ideal for incorporation into passive electronic components such as inductors and transformers, which require a non-permanent magnetic core to rapidly switch magnetization. As a result, there is a need for materials with the right combination of low coercivity, low magnetic remanence, high relative permeability, and high saturation magnetization to achieve these goals. Iron nitride is an attractive soft magnetic material for incorporation into an amine/epoxy resin matrix. This permits the synthesis of net-shaped SMCs using a “bottom-up” approach for overcoming the limitations of current state-of-the-art SMCs made via conventional powder metal processing techniques. In this work we present the fabrication of various net-shaped, iron nitride-based SMCs using two different amine/epoxy resin systems and their magnetic characterization. The maximum volume loading of iron nitride reached was ∼77% via hot pressing, which produced SMCs with a saturation magnetic polarization (Js) of ∼0.9 T, roughly 2–3 times the Js of soft ferrites.

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Phase stability and magnetic and electronic properties of a spark plasma sintered CoFe – P soft magnetic alloy

Journal of Alloys and Compounds

Belcher, Calvin H.; Zheng, Baolong; Dickens, Sara M.; Domrzalski, Jessica N.; Langlois, Eric D.; Lehman, Benjamin; Pearce, Charles J.; Delaney, Robert E.; Macdonald, Benjamin E.; Apelian, Diran; Lavernia, Enrique J.; Monson, Todd

More efficient power conversion devices are able to transmit greater electrical power across larger distances to satisfy growing global electrical needs. A critical requirement to achieve more efficient power conversion are the soft magnetic materials used as core materials in transformers, inductors, and motors. To that effect it is well known that the use of non-equilibrium microstructures, which are, for example, nanocrystalline or consist of single phase solid solutions, can yield high saturation magnetic polarization and high electrical resistivity necessary for more efficient soft magnetic materials. In this work, we synthesized CoFe – P soft magnetic alloys containing nanocrystalline, single phase solid solution microstructures and studied the effect of a secondary intermetallic phase on the saturation magnetic polarization and electrical resistivity of the consolidated alloy. Single phase solid solution CoFe – P alloys were prepared through mechanically alloying metal powders and phase decomposition was observed after subsequent consolidation via spark plasma sintering (SPS) at various temperatures. The secondary intermetallic phase was identified as the orthorhombic (CoxFe1−x)2P phase and the magnetic properties of the (CoxFe1−x)2P intermetallic phase were found to be detrimental to the soft magnetic properties of the targeted CoFe – P alloy.

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Surface Functionalized Barium Titanate Nanoparticles: A Combined Experimental and Computational Study

ECS Journal of Solid State Science and Technology

Domrzalski, Jessica N.; Stevens, Tyler E.; Van Ginhoven, Renee M.; Fritzsching, Keith; Walder, Brennan J.; Johnson, Emily M.; Lewis, Riley E.; Vreeland, Erika; Pearce, Charles J.; Vargas, David A.; Coker, Eric N.; Foulk, James W.; Grey, John K.; Monson, Todd

Barium titanate (BTO) nanoparticles show great potential for use in electrostatic capacitors with high energy density. This includes both polymer composite and sintered capacitors. However, questions about the nanoparticles’ size distribution, amount of agglomeration, and surface ligand effect on performance properties remain. Reducing particle agglomeration is a crucial step to understanding the properties of nanoscale particles, as agglomeration has significant effects on the composite dielectric constant. BTO surface functionalization using phosphonic acids is known reduce BTO nanoparticle agglomeration. We explore solution synthesized 10 nm BTO particles with tert-butylphosphonic acid ligands. Recent methods to quantifying agglomeration using an epoxy matrix before imaging shows that tert-butylphosphonic acid ligands reduce BTO agglomeration by 33%. Thermometric, spectroscopic, and computational methods provide confirmation of ligand binding and provide evidence of multiple ligand binding modes on the BTO particle surface.

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Programmable Photoluminescence via Intrinsic and DNA-Fluorophore Association in a Mixed Cluster Heterometallic MOF

ACS Applied Materials and Interfaces

Gallis, Dorina F.S.; Butler, Kimberly S.; Pearce, Charles J.; Valdez, Nichole R.; Rodriguez, Mark A.

A rapid and facile design strategy to create a highly complex optical tag with programmable, multimodal photoluminescent properties is described. This was achieved via intrinsic and DNA-fluorophore hidden signatures. As a first covert feature of the tag, an intricate novel heterometallic near-infrared (NIR)-emitting mesoporous metal-organic framework (MOF) was designed and synthesized. The material is constructed from two chemically distinct, homometallic hexanuclear clusters based on Nd and Yb. Uniquely, the Nd-based cluster is observed here for the first time in a MOF and consists of two staggered Nd μ3-oxo trimers. To generate controlled, multimodal, and tailorable emission with difficult to counterfeit features, the NIR-emissive MOF was post-synthetically modified via a fluorescent DNA oligo labeling design strategy. The surface attachment of several distinct fluorophores, including the simultaneous attachment of up to three distinct fluorescently labeled oligos was achieved, with excitation and emission properties across the visible spectrum (480-800 nm). The DNA inclusion as a secondary covert element in the tag was demonstrated via the detection of SYBR Gold dye association. Importantly, the approach implemented here serves as a rapid and tailorable way to encrypt distinct information in a facile and modular fashion and provides an innovative technology in the quest toward complex optical tags.

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The role of microstructural evolution during spark plasma sintering on the soft magnetic and electronic properties of a CoFe–Al2O3 soft magnetic composite

Journal of Materials Science

Belcher, Calvin H.; Zheng, Baolong; Macdonald, Benjamin E.; Langlois, Eric D.; Lehman, Benjamin; Pearce, Charles J.; Delaney, Robert E.; Apelian, Diran; Lavernia, Enrique J.; Monson, Todd

For transformers and inductors to meet the world’s growing demand for electrical power, more efficient soft magnetic materials with high saturation magnetic polarization and high electrical resistivity are needed. This work aimed at the development of a soft magnetic composite synthesized via spark plasma sintering with both high saturation magnetic polarization and high electrical resistivity for efficient soft magnetic cores. CoFe powder particles coated with an insulating layer of Al2O3 were used as feedstock material to improve the electrical resistivity while retaining high saturation magnetic polarization. By maintaining a continuous non-magnetic Al2O3 phase throughout the material, both a high saturation magnetic polarization, above 1.5 T, and high electrical resistivity, above 100 μΩ·m, were achieved. Through microstructural characterization of samples consolidated at various temperatures, the role of microstructural evolution on the magnetic and electronic properties of the composite was elucidated. Upon consolidation at relatively high temperature, the CoFe was to found plastically deform and flow into the Al2O3 phase at the particle boundaries and this phenomenon was attributed to low resistivity in the composite. In contrast, at lower consolidation temperatures, perforation of the Al2O3 phase was not observed and a high electrical resistivity was achieved, while maintaining a high magnetic polarization, ideal for more efficient soft magnetic materials for transformers and inductors.

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Synthesis and behavior of bulk iron nitride soft magnets via high-pressure spark plasma sintering

Journal of Materials Research

Monson, Todd; Zheng, Baolong; Delaney, Robert E.; Pearce, Charles J.; Zhou, Yizhang; Atcitty, Stanley; Lavernia, Enrique

Abstract: In this study, dense bulk iron nitrides (FexN) were synthesized for the first time ever using spark plasma sintering (SPS) of FexN powders. The Fe4N phase of iron nitride in particular has significant potential to serve as a new soft magnetic material in both transformer and inductor cores and electrical machines. The density of SPSed FexN increased with SPS temperature and pressure. The microstructure of the consolidated bulk FexN was characterized with X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and superconducting quantum interference device (SQUID) magnetometry. XRD revealed a primary phase of Fe4N with secondary phases of Fe3N and metallic iron. Finite element analysis (FEA) was also applied to investigate and explain localized heating and temperature distribution during SPS. The effects of processing on interface bonding formation and phase evolution were investigated and discussed in detail to provide insight into fundamental phenomena and microstructural evolution in SPSed FexN. Graphic abstract: [Figure not available: see fulltext.]

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Encoding Multilayer Complexity in Anti-Counterfeiting Heterometallic MOF-Based Optical Tags

Angewandte Chemie - International Edition

Deneff, Jacob I.; Butler, Kimberly S.; Rohwer, Lauren E.S.; Pearce, Charles J.; Valdez, Nichole R.; Rodriguez, Mark A.; Luk, Ting S.; Gallis, Dorina F.S.

Optical tags provide a way to quickly and unambiguously identify valuable assets. Current tag fluorophore options lack the tunability to allow combined methods of encoding in a single material. Herein we report a design strategy to encode multilayer complexity in a family of heterometallic rare-earth metal–organic frameworks based on highly connected nonanuclear clusters. To impart both intricacy and security, a synergistic approach was implemented resulting in both overt (visible) and covert (near-infrared, NIR) properties, with concomitant multi-emissive spectra and tunable luminescence lifetimes. Tag authentication is validated with a variety of orthogonal detection methodologies. Importantly, the effect induced by subtle compositional changes on intermetallic energy transfer, and thus on the resulting photophysical properties, is demonstrated. This strategy can be widely implemented to create a large library of highly complex, difficult-to-counterfeit optical tags.

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Antibody Targeted Metal-Organic Frameworks for Bioimaging Applications

ACS Applied Materials and Interfaces

Butler, Kimberly S.; Pearce, Charles J.; Nail, Elizabeth; Vincent, Grace A.; Gallis, Dorina F.S.

We report on the availability and chemical utility of primary amines within metal-organic frameworks (MOFs) for cell targeting. Primary amine groups represent one of the most versatile chemical moieties for conjugation to biologically relevant molecules, including antibodies and enzymes. Specifically, we used two different chemical conjugations schemes, utilizing the amino functionality on the organic linker: first, carbodiimide chemistry was used to link the primary amine to available carboxyl groups on the protein neutravidin; second, sulfhydryl cross-linking chemistry was used via Traut's reagent scheme. Importantly, this is the first report that documents this methodology implemented with MOF systems. Finally, the ability of the EpCAM antibody targeted MOFs to bind to a human epithelial cell line (A549), a common target for imaging studies, was confirmed with confocal microscopy.

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Results 1–25 of 54
Results 1–25 of 54