Greg Haugstad’s research while affiliated with University of Minnesota, Duluth and other places

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Publications (20)


Giant spin Hall effect with multi-directional spin components in Ni4W
  • Preprint
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November 2024

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52 Reads

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Jian-Ping Wang

Spin-orbit torque (SOT) can be used to efficiently manipulate the magnetic state of magnetic materials, which is an essential element for memory and logic applications. Due to symmetry constraints, only in-plane spins can be injected into the ferromagnet from the underlying SOT layer for conventional SOT materials such as heavy metals and topological materials. Through the use of materials with low symmetries, or other symmetry breaking approaches, unconventional spin currents with out-of-plane polarization has been demonstrated and enabled field-free deterministic switching of perpendicular magnetization. Despite this progress, the SOT efficiency of these materials has typically remained low. Here, we report a giant SOT efficiency of 0.85 in sputtered Ni4W/CoFeB heterostructure at room temperature, as evaluated by second harmonic Hall measurements. In addition, due to the low crystal symmetry of Ni4W, unconventional out-of-plane and Dresselhaus-like spin components were observed. Macro-spin simulation suggests our spin Hall tensor to provide about an order of magnitude improvement in the magnetization switching efficiency, thus broadening the path towards energy efficient spintronic devices using low-symmetry materials.

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Crystal growth, microscopy, and powder X-ray diffraction for metathesis/flux and chemical vapor transport (CVT) crystals
a Schematic of CVT growth of PdCoO2. b Scanning electron microscopy image of the products of metathesis/flux growth. Inset: Optical microscopy image of a larger single crystal from metathesis/flux growth (0.8 × 0.6 × 0.017 mm³). c Optical microscopy image of a multicrystal from CVT growth. Inset: Optical microscopy image of a typical single crystal from CVT (3.5 × 2.0 × 0.17 mm³). d, e Powder X-ray diffraction patterns (intensity vs. 2θ angle) from representative ground crystals from the metathesis/flux ((d), green) and CVT ((e), blue) methods; reference patterns are shown in gray.
Structural and chemical characterization of CVT-grown single-crystal PdCoO2
a Back-reflection Laue X-ray diffraction pattern along a [001] zone axis of a representative single crystal, with reciprocal-space axes labeled. b Corresponding simulated Laue pattern where the size of the points indicates their relative intensity and the central black circle represents the beam aperture. The simulation is based on the accepted PdCoO2 structure and lattice parameters6,79. c Specular high-resolution X-ray diffraction (intensity vs. 2θ angle) from a representative 001-oriented single crystal, showing only 00l reflections. Inset: Rocking curve through the 006 reflections in (c), with a full-width-at-half-maximum (FWHM) of 0.0089°. d Energy-dispersive X-ray spectrum (intensity vs. energy) from a representative region (25 × 25 μm²) of a single crystal. The peaks are labeled and the inset is a close-up of the 0 to 3.9 keV region shaded gray. e Particle-induced X-ray emission spectra from two crystals (CVT 1 in blue and CVT 2 in orange), along with the GUPIXWIN simulation result discussed in the text (black, vertically offset for clarity). The peaks labeled with an “*” are known instrumental artifacts in our ion beam accelerator/PIXE system. The inset is a close-up of the 4.5–7.3 keV region shaded gray; note the different intensities of the Cr and Fe Kα peaks in the two crystals. The Cr peak at 5.4 keV has partial overlap with an artifact peak but the variation in intensity from crystal to crystal strongly suggests a contribution from Cr. The Fe peak at 6.4 keV has no such overlap and also varies from crystal to crystal.
Electronic and magnetic properties of CVT-grown single-crystal PdCoO2
a a-b-plane resistivity (ρab) vs. temperature (T) on a representative single crystal. Inset: Image of the crystal and four-point in-line contact arrangement. b Data from (a) on a log10-log10 scale, highlighting the residual resistivity ratio of 436 ± 25. The error bars in (b) represent the uncertainty estimated from offset subtraction (dominant at low-T) and sample dimension measurements. c Molar magnetic susceptibility (χmol) vs. T in a 1 T magnetic field (blue open circles), from a representative powdered crystal. The black solid line is a fit to a sum of Pauli and Curie-Weiss susceptibilities, as discussed in the text. Inset: T dependence of (χmol - χ0)⁻¹, where χ0 is the T-independent susceptibility. The solid black line is a 5–20 K Curie-Weiss fit. d 2-K magnetization (M, corrected for χ0) vs. magnetic field (μ0H) for the crystal in (c) (blue open circles). The solid black line is a Brillouin fit described in the text.
Impurity analysis of CVT-grown PdCoO2
a PdCoO2 crystal structure. b Periodic table highlighting elements relevant to the delafossite structure. As in (a), light yellow highlights elements that are known to adopt the A-site in ABO2 compounds but do not fit the Pd site in PdCoO2. Dark yellow highlights elements that are known to adopt the A-site in delafossites and do fit the Pd site in PdCoO2; these are highlighted by the bold black border. Analogously, the lightest blue highlights elements that are known to adopt the B site in ABO2 compounds but do not fit the Co site in PdCoO2, and the darkest blue highlights elements that are known to adopt the B site in delafossites and do fit the Co site in PdCoO2; the intermediate blue shade highlights elements for which it is unknown whether they adopt the B site in ABO2 compounds but they do fit the Co site in PdCoO2. In this scheme, dark yellow highlights elements likely to substitute for Pd (only four), while the two darker blue colors highlight elements likely to substitute for Co (>20). Also shown for each element are the valence, coordination number, and ionic radius⁸⁰ in the state most closely relevant to delafossite oxides. (Ranges of radii are for low- to high-spin states). Au is not shaded dark yellow in (b); there exists some evidence of Au¹⁺ in linear coordination with O²⁻⁸¹ but it is uncommon. c Periodic table labeled with the detected concentration and detection limit for each element probed in mass spectrometry. All values are weight-basis ppm, averaged over multiple runs and CVT crystals, as in Tables 2–4. The color scale (right) is a log10-scale of average impurity concentration in CVT crystals. As in (b), the bold black border highlights elements likely to substitute for Pd; their total concentration is only 1.9 ppm. The entire rare-earth element block appears as “RE” in panels (b, c); in panel (c), the values are sum totals for these RE elements. Na, B, and Si, which are common glassware impurities, were excluded from ICP-MS analyses.
DFT-calculated electronic band structure and density-of-states of lightly-substituted PdCoO2
a–d Band structure of Pd1-xPtxCoO2, Pd1-xAgxCoO2, PdCo1-xFexO2, and PdCo1-xAlxO2, respectively, for x = 0.037, i.e., 3.7% substitutional impurity density. Shown is the high-symmetry k-path Γ-L-F-Γ-T, in the first Brillouin zone, with energies relative to the Fermi energy, EF. The intensities are on a log10 scale depicting the weight of the unfolded primitive cell bands obtained from the supercell bands via the unfolding method77,78. e–h Corresponding density-of-states (DOS). Shown are the total DOS (black), and the atom-projected DOS of Pd (dark yellow), Co (blue), O (red), and the respective impurity (cyan). The DOS values are for the primitive cell, calculated by dividing by the corresponding number of atoms in the supercell. The atom-projected DOS curves for the impurity atoms (labeled with an asterisk) should thus be scaled by a factor of 0.037 for direct comparison; they are plotted here unscaled for improved visibility.
Crystal-chemical origins of the ultrahigh conductivity of metallic delafossites

February 2024

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112 Reads

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11 Citations

Despite their highly anisotropic complex-oxidic nature, certain delafossite compounds (e.g., PdCoO2, PtCoO2) are the most conductive oxides known, for reasons that remain poorly understood. Their room-temperature conductivity can exceed that of Au, while their low-temperature electronic mean-free-paths reach an astonishing 20 μm. It is widely accepted that these materials must be ultrapure to achieve this, although the methods for their growth (which produce only small crystals) are not typically capable of such. Here, we report a different approach to PdCoO2 crystal growth, using chemical vapor transport methods to achieve order-of-magnitude gains in size, the highest structural qualities yet reported, and record residual resistivity ratios ( > 440). Nevertheless, detailed mass spectrometry measurements on these materials reveal that they are not ultrapure in a general sense, typically harboring 100s-of-parts-per-million impurity levels. Through quantitative crystal-chemical analyses, we resolve this apparent dichotomy, showing that the vast majority of impurities are forced to reside in the Co-O octahedral layers, leaving the conductive Pd sheets highly pure (∼1 ppm impurity concentrations). These purities are shown to be in quantitative agreement with measured residual resistivities. We thus conclude that a sublattice purification mechanism is essential to the ultrahigh low-temperature conductivity and mean-free-path of metallic delafossites.



Chondroitin sulfate is required for follicle epithelial integrity and organ shape maintenance in Drosophila

September 2023

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76 Reads

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1 Citation

Development

Heparan sulfate (HS) and chondroitin sulfate (CS) are evolutionarily conserved glycosaminoglycans that are found in most animal species, including the genetically tractable model organism Drosophila. In contrast to extensive in vivo studies elucidating co-receptor functions of Drosophila HS proteoglycans (PGs), only a limited number of studies have been conducted for those of CSPGs. To investigate the global function of CS in development, we generated mutants for Chondroitin sulfate synthase (Chsy), which encodes the Drosophila homolog of mammalian chondroitin synthase 1, a crucial CS biosynthetic enzyme. Our characterizations of the Chsy mutants indicated that a fraction survive to adult stage, which allowed us to analyze the morphology of the adult organs. In the ovary, Chsy mutants exhibited altered stiffness of the basement membrane and muscle dysfunction, leading to a gradual degradation of the gross organ structure as mutant animals aged. Our observations show that normal CS function is required for the maintenance of the structural integrity of the ECM and gross organ architecture.


Crystal-Chemical Origins of the Ultrahigh Conductivity of Metallic Delafossites

August 2023

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134 Reads

Despite their highly anisotropic complex-oxidic nature, certain delafossite compounds (e.g., PdCoO2) are the most conductive oxides known, for reasons that remain poorly understood. It is widely accepted that these materials are somehow ultrapure, although the methods for their growth (which produce only small crystals) are not typically capable of such. Here, we report a new approach to PdCoO2 crystal growth, using chemical vapor transport to achieve order-of-magnitude gains in size, the highest structural qualities reported, and record residual resistivity ratios (>440). Nevertheless, the first detailed mass spectrometry on these materials reveals that they are not ultrapure, typically harboring 100s-of-parts-per-million impurity levels. For crystal-chemical reasons that we elaborate in full, however, the majority of these impurities must reside in Co-O octahedral layers, leaving the conductive Pd sheets highly pure (~1 ppm). We thus conclude that a "sublattice purification" mechanism is essential to the ultrahigh low-temperature conductivity and mean-free-path of metallic delafossites.


Delivery of RNA to the Blood-Brain Barrier Endothelium Using Cationic Bicelles

August 2023

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149 Reads

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5 Citations

Blood-brain barrier (BBB) dysfunction is prevalent in Alzheimer’s disease and other neurological disorders. Restoring normal BBB function through RNA therapy is a potential avenue for addressing cerebrovascular changes in these disorders that may lead to cognitive decline. Although lipid nanoparticles have been traditionally used as drug carriers for RNA, bicelles have been emerging as a better alternative because of their higher cellular uptake and superior transfection capabilities. Cationic bicelles composed of DPPC/DC7PC/DOTAP at molar ratios of 63.8/25.0/11.2 were evaluated for the delivery of RNA in polarized hCMEC/D3 monolayers, a widely used BBB cell culture model. RNA-bicelle complexes were formed at five N/P ratios (1:1 to 5:1) by a thin-film hydration method. The RNA-bicelle complexes at N/P ratios of 3:1 and 4:1 exhibited optimal particle characteristics for cellular delivery. The cellular uptake of cationic bicelles laced with 1 mol% DiI-C18 was confirmed by flow cytometry and confocal microscopy. The ability of cationic bicelles (N/P ratio 4:1) to transfect polarized hCMEC/D3 with FITC-labeled control siRNA was tested vis-a-vis commercially available Lipofectamine RNAiMAX. These studies demonstrated the higher transfection efficiency and greater potential of cationic bicelles for RNA delivery to the BBB endothelium.



Precursor selection in hybrid molecular beam epitaxy of alkaline-earth stannates

December 2020

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19 Reads

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11 Citations

Journal of Vacuum Science & Technology A Vacuum Surfaces and Films

One of the challenges of oxide molecular beam epitaxy (MBE) is the synthesis of oxides containing metals with high electronegativity (metals that are hard to oxidize). The use of reactive organometallic precursors can potentially address this issue. To investigate the formation of radicals in MBE, we explored three carefully chosen metal-organic precursors of tin for SnO2 and BaSnO3 growth: tetramethyltin (TMT), tetraethyltin (TET), and hexamethylditin (HMDT). All three precursors produced single-crystalline, atomically smooth, and epitaxial SnO2 (101) films on r-Al2O3 ( 10 1 ¯ 2 ) in the presence of oxygen plasma. The study of growth kinetics revealed reaction-limited and flux-limited regimes except for TET, which also exhibited a decrease in the deposition rate with increasing temperature above ∼800 °C. Contrary to these similarities, the performance of these precursors was dramatically different for BaSnO3 growth. TMT and TET were ineffective in supplying adequate tin, whereas HMDT yielded phase-pure, stoichiometric BaSnO3 films. Significantly, HMDT resulted in phase-pure and stoichiometric BaSnO3 films even without the use of an oxygen plasma (i.e., with molecular oxygen alone). These results are discussed using the ability of HMDT to form tin radicals and therefore assisting with Sn → Sn⁴⁺ oxidation reaction. Structural and electronic transport properties of films grown using HMDT with and without oxygen plasma are compared. This study provides guideline for the choice of precursors that will enable the synthesis of metal oxides containing hard-to-oxidize metals using reactive radicals in MBE.


Citations (14)


... The wear of polymers is one of the most important mechanisms for the release of secondary micro-and nanoplastics into the environment [10,11]. Mechanical processes, such as friction, abrasion, and various shear forces, consume polymeric materials and release plastic particles from them into air, water, and soil [12,13]. ...

Reference:

On the Formation and Characterization of Nanoplastics During Surface Wear Processes
Nanoscale Abrasive Wear of Polyethylene: A Novel Approach To Probe Nanoplastic Release at the Single Asperity Level
  • Citing Article
  • June 2024

Environmental Science and Technology

... E. Maines and colleagues investigated the mechanical recycling of 3D-printed objects through the cryomilling technique. The resulting powder was incorporated into fresh resin at concentrations of up to 30% by weight, and tests conducted on newly fabricated objects demonstrated promising properties [206]. In another study, a fully renewable lipoate-based photopolymer resin was developed, allowing for the 3D printing of high-resolution objects that can be efficiently disassembled and circularly reprinted [207]. ...

Mechanical Recycling of 3D-Printed Thermosets for Reuse in Vat Photopolymerization
  • Citing Article
  • April 2024

ACS Applied Polymer Materials

... 4-8 Many of the prominently discussed triangular lattice compounds crystallize in structures related to the delafossite structure type. [8][9][10][11] Delafossite-type chromium compounds, with the general formula ACrX 2 (A = +I oxidation state metal and X = chalcogenide), consist of CrX 2 layers intercalated by the A cations in a trigonal-rhombohedral stacking. 12,13 Deintercalation of the A cations modifies the oxidation state from Cr III to Cr IV , resulting in materials with a van der Waals (vdW) gap, such as the series' end members CrTe 2 , CrSe 2 , and H x CrS 2 . ...

Crystal-chemical origins of the ultrahigh conductivity of metallic delafossites

... As a result, the transport properties primarily depend on the content and microstructure of the crystalline component, as well as on the nano-/microstructure of the amorphous component. The relationship between structure and gas barrier properties in semicrystalline polymers has been discussed for decades [4,11,[15][16][17]. To date, some studies have suggested that increasing crystallinity contributes monotonically to extending the tortuous diffusion path and reducing the sorption capacity by decreasing the content of the amorphous phase, while in others, this relationship has not been as straightforward [13,18]. ...

Polyethylene Blends for Improved Oxygen Barrier: Processing-Dependent Microstructure and Gas Permeability
  • Citing Article
  • December 2023

ACS Applied Polymer Materials

... The characterization of nano GEM adhered to the protocols established previously [24]. To illustrate the rate of intracellular uptake among nano GEM, DiI (MCE), a fluorescent dye [24,25], was implemented as a label for nano GEM. After seeding GEM-20 and CFPAC-1 cells in glass dishes for 24 h, they were incubated with DiI-labeled nano GEM over varying durations, i.e., 1, 2, 4, 6, or 8 h, with the consistent DiI concentration of 0.4 μM. ...

Delivery of RNA to the Blood-Brain Barrier Endothelium Using Cationic Bicelles

... Deforming flexible substrates transferred with 2D materials is considered a common method 25,26 but often results in limited strain magnitude due to weak van der Waals (vdW) forces at the interface 27 . Increasing research initiatives are being directed toward the creation of spatially inhomogeneous strain in 2D materials by transferring 2D materials to a non-flat substrat 28,29 . However, this method risks damaging the materials during the transfer process and suffers from uncontrollable strain magnitudes. ...

Holey Substrate-Directed Strain Patterning in Bilayer MoS 2
  • Citing Article
  • November 2021

ACS Nano

... The BSO/STaO heterostructures were generated by stacking six cubic (5 atoms) units of BSO and six cubic (5 atoms) units of STaO along the [001] direction, following previous work [16]. The cross-sectional area of the heterostructures was fixed at the ACBN0 equilibrium lattice parameter of the BSO substrate (a = 4.118 Å), following previous work [14,47], leading to an in-plane ∼1.9% tensile strain in the STaO layer. SSO/STaO interfaces were constructed using the supercells of (SSO)N/(STaO)N, where N is the number of (20 atoms) orthorhombic units of each of the two juxtaposed perovskites at the interface. ...

Precursor selection in hybrid molecular beam epitaxy of alkaline-earth stannates
  • Citing Article
  • December 2020

Journal of Vacuum Science & Technology A Vacuum Surfaces and Films

... There has been a recent trend among universities to consolidate all research infrastructure (for example, cytometry, mass spectrometry, -omics, preclinical imaging, analytical biology, microscopy) together in a centralized manner, either in one central building or in a concerted way where infrastructure is brought together and managed where the research needs arise [46]. Undoubtedly, well-managed core facilities provide the best support structure currently available in academic institutes, ensuring best practices in research, while also serving as an overall institutional cost-saving exercise [47,48]. ...

Shared instrumentation facilities: Benefiting researchers and universities, and sustaining research excellence

MRS Bulletin

... penetrates the bilayer without compromising its integrity, with the PEO providing the binding to the membranes. Collectively, these results shed light on the mechanisms underlying the membrane interactions and protective effects of P188 and related polymers, informing their potential therapeutic applications for membrane stabilization and drug delivery [90][91][92][93]. ...

Spatial Distribution of PEO–PPO–PEO Block Copolymer and PEO Homopolymer in Lipid Bilayers
  • Citing Article
  • March 2020

Langmuir

... BaXO 3 is a part of the ABO 3 class of perovskites, which are widely used in optical computer systems, pyroelectric sensors, varistors, multilayer ceramic capacitors, electro-optical devices, piezoelectric devices, and semiconductive ceramics [1]. Additionally, perovskite-based hydropower cells, which generate green electricity from strained BaTiO 3 , are a well-established, consistent, and long-lasting technology [2]. ...

Magnetism and transport in transparent high-mobility BaSnO 3 films doped with La, Pr, Nd, and Gd
  • Citing Article
  • December 2019

Physical Review Materials