Showing 1–50 of 51 results for author: Parker, D S

Constraints on magnetism and correlations in RuO$_2$ from lattice dynamics and Mössbauer spectroscopy

Authors: George Yumnam, Parul R. Raghuvanshi, John D. Budai, Dipanshu Bansal, Lars Bocklage, Douglas Abernathy, Yongqiang Cheng, Ayman Said, Igor I. Mazin, Haidong Zhou, Benjamin A. Frandsen, David S. Parker, Lucas R. Lindsay, Valentino R. Cooper, Michael E. Manley, Raphaël P. Hermann

Abstract: We provide experimental evidence for the absence of a magnetic moment in bulk RuO$_2$, a candidate altermagnetic material, by using a combination of Mössbauer spectroscopy, nuclear forward scattering, inelastic X-ray and neutron scattering, and density functional theory calculations. Using complementary Mössbauer and nuclear forward scattering we determine the $^{99}$Ru magnetic hyperfine splittin… ▽ More We provide experimental evidence for the absence of a magnetic moment in bulk RuO$_2$, a candidate altermagnetic material, by using a combination of Mössbauer spectroscopy, nuclear forward scattering, inelastic X-ray and neutron scattering, and density functional theory calculations. Using complementary Mössbauer and nuclear forward scattering we determine the $^{99}$Ru magnetic hyperfine splitting to be negligible. Inelastic X-ray and neutron scattering derived lattice dynamics of RuO$_2$ are compared to density functional theory calculations of varying flavors. Comparisons among theory with experiments indicate that electronic correlations, rather than magnetic order, are key in describing the lattice dynamics. △ Less

Submitted 6 May, 2025; originally announced May 2025.

Anomalous temperature-dependent magnetization in the nearly collinear antiferromagnet Y$_2$Co$_3$

Authors: Yunshu Shi, Huibo Cao, Hung-Cheng Wu, Li Yin, Neil Harrison, David S. Parker, Tushar Bhowmick, Tessa McNamee, Fatemeh Safari, Sergey L. Budko, James C. Fettinger, Susan M. Kauzlarich, Peter Klavins, Dmitry Popov, Ravhi Kumar, Russell J. Hemley, Shanti Deemyad, Taku J. Sato, Paul. C. Canfield, Valentin Taufour

Abstract: Y$_2$Co$_3$ is a newly discovered antiferromagnetic (AFM) compound with distorted kagome layers. Previous investigations via bulk magnetization measurements suggested a complex noncollinear magnetic behavior, with magnetic moments primarily anti-aligned along the $b$ axis and some canting towards the $ac$ plane. In this study, we report the magnetic structure of Y$_2$Co$_3$ to be an A-type AFM str… ▽ More Y$_2$Co$_3$ is a newly discovered antiferromagnetic (AFM) compound with distorted kagome layers. Previous investigations via bulk magnetization measurements suggested a complex noncollinear magnetic behavior, with magnetic moments primarily anti-aligned along the $b$ axis and some canting towards the $ac$ plane. In this study, we report the magnetic structure of Y$_2$Co$_3$ to be an A-type AFM structure with ferromagnetic (FM) interactions within the distorted kagome plane and an interplane antiferromagnetic interaction, as determined by single-crystal neutron diffraction. The magnetic moments align along the $b$ axis, with minimal canting towards the $c$ axis, at odds with the previous interpretation of bulk magnetization measurements. The magnetic moments on the two distinct Co sites are [0, -0.68(3), 0] $μ_B$ and [0, 1.25(4), 0.07(1)] $μ_B$. We attribute the previously reported "noncollinear" behavior to the considerable temperature dependence of itinerant AFM exchange interactions, induced by thermal contraction along the $b$ axis. Additionally, our examination of lattice constants through pressure studies reveals compensating effects on FM and AFM interactions, resulting in negligible pressure dependence of $T_\textrm{N}$. △ Less

Submitted 26 January, 2025; originally announced January 2025.

Journal ref: Physical Review B 110,235159 (2024)

Spin density wave and van Hove singularity in the kagome metal CeTi3Bi4

Authors: Pyeongjae Park, Brenden R. Ortiz, Milo Sprague, Anup Pradhan Sakhya, Si Athena Chen, Matthias. D. Frontzek, Wei Tian, Romain Sibille, Daniel G. Mazzone, Chihiro Tabata, Koji Kaneko, Lisa M. DeBeer-Schmitt, Matthew B. Stone, David S. Parker, German D. Samolyuk, Hu Miao, Madhab Neupane, Andrew D. Christianson

Abstract: Kagome metals with van Hove singularities near the Fermi level can host intriguing quantum phenomena such as chiral loop currents, electronic nematicity, and unconventional superconductivity. However, to our best knowledge, unconventional magnetic states driven by van Hove singularities--like spin-density waves--have not been observed experimentally in kagome metals. Here, we report the magnetic a… ▽ More Kagome metals with van Hove singularities near the Fermi level can host intriguing quantum phenomena such as chiral loop currents, electronic nematicity, and unconventional superconductivity. However, to our best knowledge, unconventional magnetic states driven by van Hove singularities--like spin-density waves--have not been observed experimentally in kagome metals. Here, we report the magnetic and electronic structure of the layered kagome metal CeTi3Bi4, where Ti kagome electronic structure interacts with a magnetic sublattice of Ce3+ Jeff = 1/2 moments. Neutron diffraction reveals an incommensurate spin-density wave ground state of the Ce3+ moments, coexisting with commensurate antiferromagnetic order across most of the temperature-field phase diagram. The commensurate component is preferentially suppressed by thermal fluctuations and magnetic field, yielding a rich phase diagram involving an intermediate single-Q spin-density wave phase. First-principles calculations and angle-resolved photoemission spectroscopy identify van Hove singularities near the Fermi level, with the observed magnetic propagation vectors connecting their high density of states, strongly suggesting a van Hove singularity-assisted spin-density wave. These findings establish kagome metals LnTi3Bi4 as a model platform where the characteristic electronic structure of the kagome lattice plays a pivotal role in magnetic order. △ Less

Submitted 12 May, 2025; v1 submitted 13 December, 2024; originally announced December 2024.

Comments: 21 pages, 4 figures, SI not included

Journal ref: Nature Communications 16, 4384 (2025)

Stability frontiers in the AM$_6$X$_6$ kagome metals: The LnNb$_6$Sn$_6$ (Ln:Ce-Lu,Y) family and density-wave transition in LuNb$_6$Sn$_6$

Authors: Brenden R. Ortiz, William R. Meier, Ganesh Pokharel, Juan Chamorro, Fazhi Yang, Shirin Mozaffari, Alex Thaler, Steven J. Gomez Alvarado, Heda Zhang, David S. Parker, German D. Samolyuk, Joseph A. M. Paddison, Jiaqiang Yan, Feng Ye, Suchismita Sarker, Stephen D. Wilson, Hu Miao, David Mandrus, Michael A. McGuire

Abstract: The kagome motif is a versatile platform for condensed matter physics, hosting rich interactions between magnetic, electronic, and structural degrees of freedom. In recent years, the discovery of a charge density wave (CDW) in the AV$_3$Sb$_5$ superconductors and structurally-derived bond density waves in FeGe and ScV$_6$Sn$_6$ have stoked the search for new kagome platforms broadly exhibiting den… ▽ More The kagome motif is a versatile platform for condensed matter physics, hosting rich interactions between magnetic, electronic, and structural degrees of freedom. In recent years, the discovery of a charge density wave (CDW) in the AV$_3$Sb$_5$ superconductors and structurally-derived bond density waves in FeGe and ScV$_6$Sn$_6$ have stoked the search for new kagome platforms broadly exhibiting density wave (DW) transitions. In this work, we evaluate the known AM$_6$X$_6$ chemistries and construct a stability diagram that summarizes the structural relationships between the $\approx$125 member family. Subsequently we introduce our discovery of the broader LnNb$_6$Sn$_6$ (Ln:Ce-Nd,Sm,Gd-Tm,Lu,Y) family of kagome metals and an analogous DW transition in LuNb$_6$Sn$_6$. Our X-ray scattering measurements clearly indicate a (1/3, 1/3, 1/3) ordering wave vector ($\sqrt{3}\times\sqrt{3}\times3$ superlattice) and diffuse scattering on half-integer $L$-planes. Our analysis of the structural data supports the ``rattling mode'' DW model proposed for ScV$_6$Sn$_6$ and paints a detailed picture of the steric interactions between the rare-earth filler element and the host Nb-Sn kagome scaffolding. We also provide a broad survey of the magnetic properties within the HfFe$_6$Ge$_6$-type LnNb$_6$Sn$_6$ members, revealing a number of complex antiferromagnetic and metamagnetic transitions throughout the family. This work integrates our new LnNb$_6$Sn$_6$ series of compounds into the broader AM$_6$X$_6$ family, providing new material platforms and forging a new route forward at the frontier of kagome metal research. △ Less

Submitted 13 March, 2025; v1 submitted 15 November, 2024; originally announced November 2024.

Intricate magnetic landscape in antiferromagnetic kagome metal TbTi$_3$Bi$_4$ and interplay with Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ (Ln: Tb-Lu) shurikagome metals

Authors: Brenden R. Ortiz, Heda Zhang, Karolina Gornicka, David S. Parker, German D. Samolyuk, Fazhi Yang, Hu Miao, Qiangsheng Lu, Robert G. Moore, Andrew F. May, Michael A. McGuire

Abstract: Here we present the discovery and characterization of the kagome metal TbTi$_3$Bi$_4$ in tandem with a new series of compounds, the Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ (Ln: Tb-Lu) shurikagome metals. We previously reported on the growth of the LnTi$_3$Bi$_4$ (Ln: La-Gd$^{3+}$, Eu$^{2+}$, Yb$^{2+}$) family, a chemically diverse and exfoliable series of kagome metals with complex and highly anisotropic magne… ▽ More Here we present the discovery and characterization of the kagome metal TbTi$_3$Bi$_4$ in tandem with a new series of compounds, the Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ (Ln: Tb-Lu) shurikagome metals. We previously reported on the growth of the LnTi$_3$Bi$_4$ (Ln: La-Gd$^{3+}$, Eu$^{2+}$, Yb$^{2+}$) family, a chemically diverse and exfoliable series of kagome metals with complex and highly anisotropic magnetism. However, unlike the La-Gd analogs, TbTi$_3$Bi$_4$ cannot be synthesized by our previous methodology due to phase competition with Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ (x$\sim$1.7-1.2). Here we discuss the phase competition between the LnTi$_3$Bi$_4$ and Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ families, helping to frame the difficulty in synthesizing LnTi$_3$Bi$_4$ compounds with small Ln species and providing a strategy to circumvent formation of Ln$_{2-x}$Ti$_{6+x}$Bi$_9$. Detailed characterization of the magnetic and electronic transport properties on single crystals of TbTi$_3$Bi$_4$ reveals a highly complex landscape of magnetic phases arising from an antiferromagnetic ground state. A series of metamagnetic transitions creates at least 5 unique magnetic phase pockets, including a 1/3 and 2/3 magnetization plateau. Further, the system exhibits an intimate connection between the magnetism and magnetotransport, exhibiting sharp switching from positive (+40%) to negative magnetoresistance (-50%). Like the LnTi$_3$Bi$_4$ kagome metals, the Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ family exhibits quasi-2D networks of titanium and chains of rare-earth. We present the structures and some basic magnetic properties of the Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ family alongside our characterization of the newly discovered TbTi$_3$Bi$_4$. △ Less

Submitted 15 July, 2024; v1 submitted 18 May, 2024; originally announced May 2024.

Evolution of highly anisotropic magnetism in the titanium-based kagome metals LnTi$_3$Bi$_4$ (Ln: La...Gd$^{3+}$, Eu$^{2+}$, Yb$^{2+}$)

Authors: Brenden R. Ortiz, Hu Miao, David S. Parker, Fazhi Yang, German D. Samolyuk, Eleanor M. Clements, Anil Rajapitamahuni, Turgut Yilmaz, Elio Vescovo, Jiaqiang Yan, Andrew F. May, Michael A. McGuire

Abstract: Here we present the family of titanium-based kagome metals of the form LnTi$_3$Bi$_4$ (Ln: La...Gd$^{3+}$, Eu$^{2+}$, Yb$^{2+}$). Single crystal growth methods are presented alongside detailed magnetic and thermodynamic measurements. The orthorhombic (Fmmm) LnTi$_3$Bi$_4$ family of compounds exhibit slightly distorted titanium-based kagome nets interwoven with zig-zag lanthanide-based (Ln) chains.… ▽ More Here we present the family of titanium-based kagome metals of the form LnTi$_3$Bi$_4$ (Ln: La...Gd$^{3+}$, Eu$^{2+}$, Yb$^{2+}$). Single crystal growth methods are presented alongside detailed magnetic and thermodynamic measurements. The orthorhombic (Fmmm) LnTi$_3$Bi$_4$ family of compounds exhibit slightly distorted titanium-based kagome nets interwoven with zig-zag lanthanide-based (Ln) chains. Crystals are easily exfoliated parallel to the kagome sheets and angular resolved photoemission (ARPES) measurements highlight the intricacy of the electronic structure in these compounds, with Dirac points existing at the Fermi level. The magnetic properties and the associated anisotropy emerge from the quasi-1D zig-zag chains of Ln, and impart a wide array of magnetic ground states ranging from anisotropic ferromagnetism to complex antiferromagnetism with a cascade of metamagnetic transitions. Kagome metals continue to provide a rich direction for the exploration of magnetic, topologic, and highly correlated behavior. Our work here introduces the LnTi$_3$Bi$_4$ compounds to augment the continuously expanding suite of complex and interesting kagome materials. △ Less

Submitted 6 September, 2023; v1 submitted 30 August, 2023; originally announced August 2023.

Multiple Incommensurate Magnetic States in the Kagome Antiferromagnet Na2Mn3Cl8

Authors: Joseph A. M. Paddison, Li Yin, Keith M. Taddei, Malcolm J. Cochran, Stuart A. Calder, David S. Parker, Andrew F. May

Abstract: The kagome lattice can host exotic magnetic phases arising from frustrated and competing magnetic interactions. However, relatively few insulating kagome materials exhibit incommensurate magnetic ordering. Here, we present a study of the magnetic structures and interactions of antiferromagnetic Na$_2$Mn$_3$Cl$_8$ with an undistorted Mn$^{2+}$ kagome network. Using neutron-diffraction and bulk magn… ▽ More The kagome lattice can host exotic magnetic phases arising from frustrated and competing magnetic interactions. However, relatively few insulating kagome materials exhibit incommensurate magnetic ordering. Here, we present a study of the magnetic structures and interactions of antiferromagnetic Na$_2$Mn$_3$Cl$_8$ with an undistorted Mn$^{2+}$ kagome network. Using neutron-diffraction and bulk magnetic measurements, we show that Na$_2$Mn$_3$Cl$_8$ hosts two different incommensurate magnetic states, which develop at $T_{N1} = 1.6$ K and $T_{N2} = 0.6$ K. Magnetic Rietveld refinements indicate magnetic propagation vectors of the form $\mathbf{q} = (q_{x},q_{y},\frac{3}{2})$, and our neutron-diffraction data can be well described by cycloidal magnetic structures. By optimizing exchange parameters against magnetic diffuse-scattering data, we show that the spin Hamiltonian contains ferromagnetic nearest-neighbor and antiferromagnetic third-neighbor Heisenberg interactions, with a significant contribution from long-ranged dipolar coupling. This experimentally-determined interaction model is compared with density-functional-theory simulations. Using classical Monte Carlo simulations, we show that these competing interactions explain the experimental observation of multiple incommensurate magnetic phases and may stabilize multi-$\mathbf{q}$ states. Our results expand the known range of magnetic behavior on the kagome lattice. △ Less

Submitted 17 April, 2023; originally announced April 2023.

Comments: 13 pages, 8 figures

Field Tunable Magnetic Transitions of CsCo2(MoO4)2(OH): A Triangular Chain Structure with a Frustrated Geometry

Authors: Liurukara D Sanjeewa, V. Ovidiu Garlea, Randy S. Fishman, Mahsa Foroughian, Li Yin, Jie Xing, David S. Parker, Tiffany M. Smith Pellizzeri, Athena S. Sefat, Joseph W. Kolis

Abstract: Identifying and characterizing new magnetic systems with Co2+ ions can enhance our understanding of quantum behavior since Co2+ can host a pseudospin-1/2 magnetic ground state. Understanding the magnetic ground state and the phase diagrams of such systems are central to the development of new theoretical models to described emergent quantum properties of complex magnetic systems. The sawtooth chai… ▽ More Identifying and characterizing new magnetic systems with Co2+ ions can enhance our understanding of quantum behavior since Co2+ can host a pseudospin-1/2 magnetic ground state. Understanding the magnetic ground state and the phase diagrams of such systems are central to the development of new theoretical models to described emergent quantum properties of complex magnetic systems. The sawtooth chain compound, CsCo2MoO4_2OH, is one such complex magnetic system and here, we present a comprehensive series of magnetic and neutron scattering measurements to determine its magnetic phase diagram. The magnetic properties of CsCo2MoO4_2OH exhibit a strong coupling to the crystal lattice and its magnetic ground state can be easily manipulated by applied magnetic fields. There are two unique Co2+ ions, base and vertex, with Jbb and Jbv magnetic exchange. The magnetism is highly anisotropic with the b-axis (chain) along the easy axis and the material orders antiferromagnetically at TN = 5 K. The zero field antiferromagnetic phase contains vertex magnetic vectors Co1 aligned parallel to the b-axis, while the base vectors Co2 are canted by 34 and aligned in an opposite direction to the vertex vectors. The spins in parallel adjacent chains align in opposite directions, creating an overall antiferromagnetic structure. At a 3 kOe applied magnetic field, adjacent chains flip by 180° to generate a ferrimagnetic phase. An increase in field gradually induces the Co(1) moment to rotate along the b-axis and align in the same direction with Co2 generating a ferromagnetic structure. Our results demonstrate that the CsCo2MoO4_2OH is a promising candidate to study new physics associated with sawtooth chain magnetism. △ Less

Submitted 13 November, 2022; originally announced November 2022.

NaCo2(SeO3)2(OH): Competing Magnetic Ground States of a New Sawtooth Structure with 3d7 Co2+ Ions

Authors: Liurukara D. Sanjeewa, V. Ovidiu Garlea, Keith M. Taddei, Li Yin, Jie Xing, Randy S. Fishman, David S. Parker, Athena S. Sefat

Abstract: While certain magnetic sublattices have long been known theoretically to give rise to emergent physics via competing magnetic interactions and quantum effects, finding such configurations in real materials is often deeply challenging. Here we report the synthesis and characterization of a new such material, NaCo2(SeO3)2(OH) which crystallizes with a highly frustrated sublattice of sawtooth Co2+ ch… ▽ More While certain magnetic sublattices have long been known theoretically to give rise to emergent physics via competing magnetic interactions and quantum effects, finding such configurations in real materials is often deeply challenging. Here we report the synthesis and characterization of a new such material, NaCo2(SeO3)2(OH) which crystallizes with a highly frustrated sublattice of sawtooth Co2+ chains. Single crystals of NaCo2(SeO3)2(OH) were synthesized using a low-temperature hydrothermal method. X-ray single crystal structure analysis reveals that the material crystallizes in orthorhombic space group of Pnma (no. 62). Its crystal structure exhibits one-dimensional chains of corner-sharing isosceles triangles that are made of two crystallographically distinct 3d7 Co2+ sites (Co(1) and Co(2)). The chains run along the b-axis and are interconnected via [SeO3] groups to form a three-dimensional structure mediating super-exchange interactions. The temperature dependent magnetization data show a ferromagnetic-like (FM) transition at 11 K (T1) followed by an antiferromagnetic (AFM) transition at about 6 K (T2). Neutron-powder diffraction measurements reveal that at T1 = 11 K only Co(2) site orders magnetically, forming ferromagnetic zigzag chains along the b-axis. Below T2 = 6 K, both Co(1) and Co(2) sites order in an nearly orthogonal configuration, with Co(1) moments lying inside the plane of the sawtooth chain while Co(2) moments cant out of the plane. The canting of the magnetic moments leads to a net ferromagnetic component along b-axis, parallel to the chain direction. The ordered moments are fully compensated in the ac-plane. △ Less

Submitted 13 July, 2022; originally announced July 2022.

Comments: N/A

MSC Class: N/A

Nanometric modulations of the magnetic structure of the element Nd

Authors: H. Suriya Arachchige, L. M. DeBeer-Schmitt, L. L. Kish, Binod K. Rai, A. F. May, D. S. Parker, G. Pokharel, Wei Tian, D. G. Mandrus, M. Bleuel, Z. Islam, G. Fabbris, H. X. Li, S. Gao, H. Miao, S. M. Thomas, P. F. S. Rosa, J. D. Thompson, Shi-Zeng Lin, A. D. Christianson

Abstract: The rare earth neodymium arguably exhibits the most complex magnetic ordering and series of magnetic phase transitions of the elements. Here we report the results of small-angle neutron scattering (SANS) measurements as a function of temperature and applied magnetic field to study magnetic correlations on nanometer length scales in Nd. The SANS measurements reveal the presence of previously unrepo… ▽ More The rare earth neodymium arguably exhibits the most complex magnetic ordering and series of magnetic phase transitions of the elements. Here we report the results of small-angle neutron scattering (SANS) measurements as a function of temperature and applied magnetic field to study magnetic correlations on nanometer length scales in Nd. The SANS measurements reveal the presence of previously unreported modulation vectors characterizing the ordered spin configuration which exhibit changes in magnitude and direction that are phase dependent. Between 5.9 and 7.6 K the additional modulation vector has a magnitude $Q$ =0.12 Å$^{-1}$ and is primarily due to order of the Nd layers which contain a center of inversion. In this region of the phase diagram, the SANS measurements also identify a phase boundary at $\approx$1 T. An important feature of these modulation vectors is that they indicate the presence of nanometer length scale spin textures which are likely stabilized by frustrated Ruderman-Kittel-Kasuya-Yosida (RKKY) interactions rather than a Dzyaloshinskii-Moriya (DM) exchange interaction. △ Less

Submitted 6 July, 2022; originally announced July 2022.

Comments: 16 pages, 15 figures

Flat-Band Itinerant Antiferromagnetism in the Kagome Metal CoSn1-xInx

Authors: B. C. Sales, W. R. Meier, D. S. Parker, L. Yin, J. Q. Yan, A. F. May, S. Calder, A. A. Aczel, Q. Zhang, H. Li, T. Yilmaz, E. Vescovo, H. Miao, R. P. Hermann, M. A. McGuire

Abstract: Destructive interference of electron hopping on the frustrated kagome lattice generates Dirac nodes, saddle points, and flat bands in the electronic structure. The latter provides the narrow bands and a peak in the density of states that can generate correlated electron behavior when the Fermi level lies within them. In the kagome metal CoSn, this alignment is not realized, and the compound is a P… ▽ More Destructive interference of electron hopping on the frustrated kagome lattice generates Dirac nodes, saddle points, and flat bands in the electronic structure. The latter provides the narrow bands and a peak in the density of states that can generate correlated electron behavior when the Fermi level lies within them. In the kagome metal CoSn, this alignment is not realized, and the compound is a Pauli paramagnet. Here we show that replacing part of the tin with indium (CoSn1-xInx) moves the Fermi energy into the flat band region, with support from band structure calculations, heat capacity measurements, and angle resolved photoemission spectroscopy. The associated instability results in the emergence of itinerant antiferromagnetism with a Neel temperature up to 30K. Long range magnetic order is confirmed by neutron diffraction measurements, which indicate an ordered magnetic moment of 0.1-0.2 Bohr magnetons per Co (for x = 0.4). Thus, CoSn1-xInx provides a rare example of an itinerant antiferromagnet with a small ordered moment. This work provides clear evidence that flat bands arising from frustrated lattices in bulk crystals represent a viable route to new physics, evidenced here by the emergence of magnetic order upon introducing a non-magnetic dopant into a non-magnetic kagome metal. △ Less

Submitted 28 January, 2022; originally announced January 2022.

Journal ref: Chemistry of Materials 34, 7069 (2024)

Robust antiferromagnetism in Y$_2$Co$_3$

Authors: Yunshu Shi, David S. Parker, Eun Sang Choi, Kasey P. Devlin, Li Yin, Jingtai Zhao, Peter Klavins, Susan M. Kauzlarich, Valentin Taufour

Abstract: We report on a solution-growth based method to synthesise single crystals of Y$_2$Co$_3$ and on its structural and magnetic properties. We find that Y$_2$Co$_3$ crystallizes in the La2Ni3-type orthorhombic structure with space group Cmce (No. 64), with Co forming distorted kagome lattices. Y$_2$Co$_3$ orders antiferromagnetically below $T_N$ = 252 K. Magnetization measurements reveal that the mome… ▽ More We report on a solution-growth based method to synthesise single crystals of Y$_2$Co$_3$ and on its structural and magnetic properties. We find that Y$_2$Co$_3$ crystallizes in the La2Ni3-type orthorhombic structure with space group Cmce (No. 64), with Co forming distorted kagome lattices. Y$_2$Co$_3$ orders antiferromagnetically below $T_N$ = 252 K. Magnetization measurements reveal that the moments are primarily aligned along the b axis with evidence for some canting. Band-structure calculations indicate that ferromagnetic and antiferromagnetic orders are nearly degenerate, at odds with experimental results. Magnetization measurements under pressure up to 1 GPa reveal that the N/'eel temperature decreases with the slope of -1.69 K/GPa. We observe a field-induced spin-flop transition in the magnetization measurements at 1.5 K and 21 T with magnetic field along the b direction. The magnetization is not saturated up to 35 T, indicating that the antiferromagnetic ordering in Y$_2$Co$_3$ is quite robust, which is surprising for such a Co-rich intermetallic. △ Less

Submitted 27 January, 2022; originally announced January 2022.

Journal ref: Physical Review B 104, 184407 (2021)

Disentangling Electronic, Lattice and Spin Dynamics in the Chiral Helimagnet Cr1/3NbS2

Authors: N. Sirica, H. Hedayat, D. Bugini, M. R. Koehler, L. Li, D. S. Parker, D. G. Mandrus, C. Dallera, E. Carpene, N. Mannella

Abstract: We investigate the static and ultrafast magneto-optical response of the hexagonal chiral helimagnet $Cr_{1/3}NbS_{2}$ above and below the helimagnetic ordering temperature. The presence of a magnetic easy plane contained within the crystallographic ab-plane is confirmed, while degenerate optical pump-probe experiments reveal significant differences in the dynamic between the parent, $NbS_{2}$, and… ▽ More We investigate the static and ultrafast magneto-optical response of the hexagonal chiral helimagnet $Cr_{1/3}NbS_{2}$ above and below the helimagnetic ordering temperature. The presence of a magnetic easy plane contained within the crystallographic ab-plane is confirmed, while degenerate optical pump-probe experiments reveal significant differences in the dynamic between the parent, $NbS_{2}$, and Cr-intercalated compounds. Time resolved magneto-optical Kerr effect measurements show a two-step demagnetization process, where an initial, sub-ps relaxation and subsequent buildup ($τ> 50$ ps) in the demagnetization dynamic scale similarly with increasing pump fluence. Despite theoretical evidence for partial gapping of the minority spin channel, suggestive of possible half metallicity in $Cr_{1/3}NbS_{2}$, such a long demagnetization dynamic likely results from spin lattice-relaxation as opposed to minority state blocking. However, comparison of the two-step demagnetization process in $Cr_{1/3}NbS_{2}$ with other 3d intercalated transition metal dichalcogenides reveals a behavior that is unexpected from conventional spin-lattice relaxation, and may be attributed to the complicated interaction of local moments with itinerant electrons in this material system. △ Less

Submitted 22 November, 2021; originally announced November 2021.

Comments: 20 pages, 10 figures, 1 Table

Journal ref: Phys. Rev. B 104, 174426 (2021)

Witnessing quantum criticality and entanglement in the triangular antiferromagnet KYbSe$_2$

Authors: A. O. Scheie, E. A. Ghioldi, J. Xing, J. A. M. Paddison, N. E. Sherman, M. Dupont, L. D. Sanjeewa, Sangyun Lee, A. J. Woods, D. Abernathy, D. M. Pajerowski, T. J. Williams, Shang-Shun Zhang, L. O. Manuel, A. E. Trumper, C. D. Pemmaraju, A. S. Sefat, D. S. Parker, T. P. Devereaux, R. Movshovich, J. E. Moore, C. D. Batista, D. A. Tennant

Abstract: The Heisenberg triangular lattice quantum spin liquid and the phase transitions to nearby magnetic orders have received much theoretical attention, but clear experimental manifestations of these states are rare. This work investigates a new spin-half Yb$^{3+}$ delafossite material, KYbSe$_2$, whose inelastic neutron scattering spectra reveal a diffuse continuum with a sharp lower bound. Applying e… ▽ More The Heisenberg triangular lattice quantum spin liquid and the phase transitions to nearby magnetic orders have received much theoretical attention, but clear experimental manifestations of these states are rare. This work investigates a new spin-half Yb$^{3+}$ delafossite material, KYbSe$_2$, whose inelastic neutron scattering spectra reveal a diffuse continuum with a sharp lower bound. Applying entanglement witnesses to the data reveals significant multipartite entanglement spread between its neighbors, and analysis of its magnetic exchange couplings shows close proximity to the triangular lattice Heisenberg quantum spin liquid. Key features of the data are reproduced by Schwinger-boson theory and tensor network calculations with a significant second-neighbor coupling $J_2$. The strength of the dynamical structure factor at the $K$ point shows a scaling collapse in $\hbarω/k_\mathrm{B}T$ down to 0.3 K, indicating a second-order quantum phase transition. Comparing this to previous theoretical work suggests that the proximate phase at larger $J_2$ is a gapped $\mathbb{Z}_2$ spin liquid, resolving a long-debated issue. We thus show that KYbSe$_2$ is close to a spin liquid phase, which in turn sheds light on the theoretical phase diagram itself. △ Less

Submitted 10 March, 2023; v1 submitted 23 September, 2021; originally announced September 2021.

Comments: 6 pages main text, 6 pages methods, 7 pages supplemental information

Journal ref: Nature Physics (2023)

Relationship between A-site Cation and Magnetic Structure in 3d-5d-4f Double Perovskite Iridates Ln2NiIrO6 (Ln=La, Pr, Nd)

Authors: T. Ferreira, S. Calder, D. S. Parker, M. H. Upton, A. S. Sefat, H. -C. zur Loye

Abstract: We report a comprehensive investigation of Ln2NiIrO6 (Ln = La, Pr, Nd) using thermodynamic and transport properties, neutron powder diffraction, resonant inelastic x-ray scattering, and density functional theory (DFT) calculations to investigate the role of A-site cations on the magnetic interactions in this family of hybrid 3d-5d-4f compositions. Magnetic structure determination using neutron dif… ▽ More We report a comprehensive investigation of Ln2NiIrO6 (Ln = La, Pr, Nd) using thermodynamic and transport properties, neutron powder diffraction, resonant inelastic x-ray scattering, and density functional theory (DFT) calculations to investigate the role of A-site cations on the magnetic interactions in this family of hybrid 3d-5d-4f compositions. Magnetic structure determination using neutron diffraction reveals antiferromagnetism for La2NiIrO6, a collinear ferrimagnetic Ni/Ir state that is driven to long range antiferromagnetism upon the onset of Nd ordering in Nd2NiIrO6, and a non-collinear ferrimagnetic Ni/Ir sublattice interpenetrated by a ferromagnetic Pr lattice for Pr2NiIrO6. For Pr2NiIrO6 heat capacity results reveal the presence of two independent magnetic sublattices and transport resistivity indicates insulating behavior and a conduction pathway that is thermally mediated. First principles DFT calculation elucidates the existence of the two independent magnetic sublattices within Pr2NiIrO6 and offers insight into the behavior in La2NiIrO6 and Nd2NiIrO6. Resonant inelastic x-ray scattering is consistent with spin-orbit coupling splitting the t2g manifold of octahedral Ir4+ into a Jeff = 1/2 and Jeff = 3/2 state for all members of the series considered. △ Less

Submitted 3 June, 2021; originally announced June 2021.

Hierarchical excitations from correlated spin tetrahedra on the breathing pyrochlore lattice

Authors: Shang Gao, Andrew F. May, Mao-Hua Du, Joseph A. M. Paddison, Hasitha Suriya Arachchige, Ganesh Pokharel, Clarina dela Cruz, Qiang Zhang, Georg Ehlers, David S. Parker, David G. Mandrus, Matthew B. Stone, Andrew D. Christianson

Abstract: The hierarchy of the coupling strengths in a physical system often engenders an effective model at low energies where the decoupled high-energy modes are integrated out. Here, using neutron scattering, we show that the spin excitations in the breathing pyrochlore lattice compound CuInCr$_4$S$_8$ are hierarchical and can be approximated by an effective model of correlated tetrahedra at low energies… ▽ More The hierarchy of the coupling strengths in a physical system often engenders an effective model at low energies where the decoupled high-energy modes are integrated out. Here, using neutron scattering, we show that the spin excitations in the breathing pyrochlore lattice compound CuInCr$_4$S$_8$ are hierarchical and can be approximated by an effective model of correlated tetrahedra at low energies. At higher energies, intra-tetrahedron excitations together with strong magnon-phonon couplings are observed, which suggests the possible role of the lattice degree of freedom in stabilizing the spin tetrahedra. Our work illustrates the spin dynamics in CuInCr$_4$S$_8$ and demonstrates a general effective-cluster approach to understand the dynamics on the breathing-type lattices. △ Less

Submitted 28 January, 2021; originally announced January 2021.

Comments: 11 pages, 9 figures

Journal ref: Phys. Rev. B 103, 214418 (2021)

Simulating Spin Waves in Entropy Stabilized Oxides

Authors: Tom Berlijn, Gonzalo Alvarez, David S. Parker, Raphaël P. Hermann, Randy S. Fishman

Abstract: The entropy stabilized oxide Mg$_{0.2}$Co$_{0.2}$Ni$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$O exhibits antiferromagnetic order and magnetic excitations, as revealed by recent neutron scattering experiments. This observation raises the question of the nature of spin wave excitations in such disordered systems. Here, we investigate theoretically the magnetic ground state and the spin-wave excitations using linea… ▽ More The entropy stabilized oxide Mg$_{0.2}$Co$_{0.2}$Ni$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$O exhibits antiferromagnetic order and magnetic excitations, as revealed by recent neutron scattering experiments. This observation raises the question of the nature of spin wave excitations in such disordered systems. Here, we investigate theoretically the magnetic ground state and the spin-wave excitations using linear spin-wave theory in combination with the supercell approximation to take into account the extreme disorder in this magnetic system. We find that the experimentally observed antiferromagnetic structure can be stabilized by a rhombohedral distortion together with large second nearest neighbor interactions. Our calculations show that the spin-wave spectrum consists of a well-defined low-energy coherent spectrum in the background of an incoherent continuum that extends to higher energies. △ Less

Submitted 2 November, 2020; originally announced November 2020.

Journal ref: Phys. Rev. Research 3, 033273 (2021)

The nature of ferromagnetism in the chiral helimagnet $Cr_{1/3}NbS_{2}$

Authors: N. Sirica, P. Vilmercati, F. Bondino, I. Pis, S. Nappini, S. -K. Mo, A. V. Fedorov, P. K. Das, I. Vobornik, J. Fujii, L. Li, D. Sapkota, D. S. Parker, D. G. Mandrus, N. Mannella

Abstract: The chiral helimagnet, $Cr_{1/3}NbS_{2}$, hosts exotic spin textures, whose influence on the magneto-transport properties, make this material an ideal candidate for future spintronic applications. To date, the interplay between macroscopic magnetic and transport degrees of freedom is believed to result from a reduction in carrier scattering following spin order. Here, we present electronic structu… ▽ More The chiral helimagnet, $Cr_{1/3}NbS_{2}$, hosts exotic spin textures, whose influence on the magneto-transport properties, make this material an ideal candidate for future spintronic applications. To date, the interplay between macroscopic magnetic and transport degrees of freedom is believed to result from a reduction in carrier scattering following spin order. Here, we present electronic structure measurements through the helimagnetic transition temperature, $T_{C}$ that challenges this view by showing a Fermi surface comprised of strongly hybridized Nb- and Cr- derived electronic states, and spectral weight in proximity to the Fermi level to anomalously increases as temperature is lowered below $T_{C}$. These findings are rationalized on the basis of first principle, density functional theory calculations, which reveal a large nearest-neighbor exchange energy, suggesting the interaction between local spin moments and hybridized Nb- and Cr- derived itinerant states to go beyond the perturbative interaction of Ruderman-Kittel-Kasuya-Yosida, suggesting instead a mechanism rooted in a Hund's exchange interaction. △ Less

Submitted 17 August, 2020; originally announced August 2020.

Journal ref: Communications Physics 3, 65 (2020)

Van Hove singularity in the magnon spectrum of the antiferromagnetic quantum honeycomb lattice

Authors: G. Sala, M. B. Stone, Binod K. Rai, A. F. May, Pontus Laurell, V. O. Garlea, N. P. Butch, M. D. Lumsden, G. Ehlers, G. Pokharel, D. Mandrus, D. S. Parker, S. Okamoto, Gábor B. Halász, A. D. Christianson

Abstract: The magnetic excitation spectrum of the quantum magnet YbCl$_3$ is studied with inelastic neutron scattering. The spectrum exhibits an unusually sharp feature within a broad continuum, as well as conventional spin waves. By including both transverse and longitudinal channels of the neutron response, linear spin wave theory with a single Heisenberg interaction on the honeycomb lattice reproduces al… ▽ More The magnetic excitation spectrum of the quantum magnet YbCl$_3$ is studied with inelastic neutron scattering. The spectrum exhibits an unusually sharp feature within a broad continuum, as well as conventional spin waves. By including both transverse and longitudinal channels of the neutron response, linear spin wave theory with a single Heisenberg interaction on the honeycomb lattice reproduces all of the key features in the spectrum. In particular, the broad continuum corresponds to a two-magnon contribution from the longitudinal channel, while the sharp feature within this continuum is identified as a Van Hove singularity in the joint density of states, which indicates the two-dimensional nature of the two-magnon continuum. We term these singularities magneto-caustic features in analogy with caustic features in ray optics where focused envelopes of light are generated when light passes through or reflects from curved or distorted surfaces. The experimental demonstration of a sharp Van Hove singularity in a two-magnon continuum is important because analogous features in potential two-spinon continua could distinguish quantum spin liquids from merely disordered systems. These results establish YbCl$_3$ as a nearly ideal two-dimensional honeycomb lattice material hosting strong quantum effects in the unfrustrated limit. △ Less

Submitted 3 March, 2020; originally announced March 2020.

Comments: 17 pages, 5 figures

Journal ref: Nature Communications 12, 171 (2021)

Cluster Frustration in the Breathing Pyrochlore Magnet LiGaCr4S8

Authors: Ganesh Pokharel, Hasitha Suriya Arachchige, Travis J. Williams, Andrew F. May, Randy S. Fishman, Gabriele Sala, Stuart Calder, Georg Ehlers, David S. Parker, Tao Hong, Andrew Wildes, David Mandrus, Joseph A. M. Paddison, Andrew D. Christianson

Abstract: We present a comprehensive neutron scattering study of the breathing pyrochlore magnet LiGaCr4S8. We observe an unconventional magnetic excitation spectrum with a separation of high and low-energy spin dynamics in the correlated paramagnetic regime above a spin-freezing transition at 12(2) K. By fitting to magnetic diffuse-scattering data, we parameterize the spin Hamiltonian. We find that interac… ▽ More We present a comprehensive neutron scattering study of the breathing pyrochlore magnet LiGaCr4S8. We observe an unconventional magnetic excitation spectrum with a separation of high and low-energy spin dynamics in the correlated paramagnetic regime above a spin-freezing transition at 12(2) K. By fitting to magnetic diffuse-scattering data, we parameterize the spin Hamiltonian. We find that interactions are ferromagnetic within the large and small tetrahedra of the breathing pyrochlore lattice, but antiferromagnetic further-neighbor interactions are also essential to explain our data, in qualitative agreement with density-functional theory predictions [Ghoshet al.,npj Quantum Mater.4, 63 (2019)]. We explain the origin of geometrical frustration in LiGaCr4S8 interms of net antiferromagnetic coupling between emergent tetrahedral spin clusters that occupy a face-centered lattice. Our results provide insight into the emergence of frustration in the presence of strong further-neighbor couplings, and a blueprint for the determination of magnetic interactions in classical spin liquids. △ Less

Submitted 22 February, 2020; originally announced February 2020.

Comments: Supplemental information available upon request

Journal ref: Phys. Rev. Lett. 125, 167201 (2020)

Superconductivity with Tc=7 K under pressure for Cu-, and Au-doped BaFe2As2

Authors: L. Li, D. S. Parker, Z. Gai, H. B. Cao, A. S. Sefat

Abstract: It is noteworthy that chemical substitution of BaFe2As2 (122) with the noble elements Cu and Au gives superconductivity with a maximum Tc=3 K, while Ag substitution (Ag-122) stays antiferromagnetic. For Ba(Fe1-xTMx)2As2, TM= Cu, Au, or Ag, and by doping an amount of x=0.04, a-lattice parameter slightly increases (0.4%) for all TM dopants, while c-lattice decreases (-0.2%) for TM=Cu, barely moves (… ▽ More It is noteworthy that chemical substitution of BaFe2As2 (122) with the noble elements Cu and Au gives superconductivity with a maximum Tc=3 K, while Ag substitution (Ag-122) stays antiferromagnetic. For Ba(Fe1-xTMx)2As2, TM= Cu, Au, or Ag, and by doping an amount of x=0.04, a-lattice parameter slightly increases (0.4%) for all TM dopants, while c-lattice decreases (-0.2%) for TM=Cu, barely moves (0.05%) for Au, and increases (0.2%) for Ag. Despite the naive expectation that the noble elements of group 11 should affect the quantum properties of 122 similarly, they produce significant differences extending to the character of the ground state. For the Ag-122 crystal, evidence of only a filamentary superconductivity is noted with pressure. However, for Au and Cu doping (x=0.03) we find a substantial improvement in the superconductivity, with Tc increasing to 7 K and 7.5 K, respectively, under 20 kbar of pressure. As with the ambient pressure results, the identity of the dopant therefore has a substantial impact on the ground state properties. Density functional theory calculations corroborate these results and find evidence of strong electronic scattering for Au and Ag dopants, while Cu is comparatively less disruptive to the 122 electronic structure. △ Less

Submitted 11 February, 2020; originally announced February 2020.

Competitive and Cooperative electronic states in Ba(Fe$_{1-x}$T$_x$)$_2$As$_2$ with T=Co, Ni, Cr

Authors: Qiang Zou, Mingming Fu, Zhiming Wu, Li Li, David S. Parker, Athena S. Sefat, Zheng Gai

Abstract: The electronic structure inhomogeneities in Co, Ni, and Cr doped BaFe2As2 122 single crystals are compared using scanning tunneling microscopy/spectroscopy (STM/S) at the nanoscale within three bulk property regions in the phase diagram: a pure superconducting (SC) dome region (Co-122), a coexisting SC and antiferromagnetic (AFM) region (Ni-122), and a non-SC region (Cr-122). Machine learning is u… ▽ More The electronic structure inhomogeneities in Co, Ni, and Cr doped BaFe2As2 122 single crystals are compared using scanning tunneling microscopy/spectroscopy (STM/S) at the nanoscale within three bulk property regions in the phase diagram: a pure superconducting (SC) dome region (Co-122), a coexisting SC and antiferromagnetic (AFM) region (Ni-122), and a non-SC region (Cr-122). Machine learning is utilized to categorize the various nanometer scale inhomogeneous electronic states, described here as in-gap, L-shape and S-shape states immersed into the SC matrix for Ni-and Co-doped 122, and L-shape and S-shape states into the metallic matrix for Cr-doped 122. Although the relative percentages of in-gap, L-shape and S-shape states vary in the three samples, the total volume fraction of the three electronic states is quite similar. This is coincident with the number of electrons (Ni0.04 and Co0.08) and holes (Cr0.04) doped into the 122 compound. By combining the volume fractions of the three states, the local density of states (LDOS), magnetic field dependent behavior and global properties in these three samples, the in-gap state is confirmed as a magnetic impurity state from the Co or Ni dopants. In addition, the L-shape state is identified as a spin density wave (SDW) which competes with the SC phase, and the S-shape state is found to be another form of magnetic order which constructively cooperates with the SC phase, rather than competing with it. The comparison of the vortex structures indicates that the inhomogeneous electronic states serve as pinning centers for stabilizing the vortex lattice. △ Less

Submitted 13 August, 2021; v1 submitted 21 August, 2019; originally announced August 2019.

Crystal field splitting, local anisotropy, and low energy excitations in the quantum magnet YbCl$_3$

Authors: G. Sala, M. B. Stone, Binod K. Rai, A. F. May, D. S. Parker, Gábor B. Halász, Y. Q. Cheng, G. Ehlers, V. O. Garlea, Q. Zhang, M. D. Lumsden, A. D. Christianson

Abstract: We study the correlated quantum magnet, YbCl$_3$, with neutron scattering, magnetic susceptibility, and heat capacity measurements. The crystal field Hamiltonian is determined through simultaneous refinements of the inelastic neutron scattering and magnetization data. The ground state doublet is well isolated from the other crystal field levels and results in an effective spin-1/2 system with loca… ▽ More We study the correlated quantum magnet, YbCl$_3$, with neutron scattering, magnetic susceptibility, and heat capacity measurements. The crystal field Hamiltonian is determined through simultaneous refinements of the inelastic neutron scattering and magnetization data. The ground state doublet is well isolated from the other crystal field levels and results in an effective spin-1/2 system with local easy plane anisotropy at low temperature. Cold neutron spectroscopy shows low energy excitations that are consistent with nearest neighbor antiferromagnetic correlations of reduced dimensionality. △ Less

Submitted 24 July, 2019; originally announced July 2019.

Comments: main paper plus supplemental information

Journal ref: Phys. Rev. B 100, 180406 (2019)

Suppression of the antiferromagnetic metallic state in the pressurized MnBi2Te4 single crystal

Authors: K. Y. Chen, B. S. Wang, J. -Q. Yan, D. S. Parker, J. -S. Zhou, Y. Uwatoko, J. -G. Cheng

Abstract: MnBi2Te4 has attracted tremendous research interest recently as the first intrinsic antiferromagnetic (AF) topological insulator. It undergoes a long-range AF order at TN = 24 K accompanied with a cusp-like anomaly in the metallic resistivity. Here, we studied the effect of hydrostatic pressure on its electrical transport properties up to 12.5 GPa by using a cubic anvil cell apparatus. We find tha… ▽ More MnBi2Te4 has attracted tremendous research interest recently as the first intrinsic antiferromagnetic (AF) topological insulator. It undergoes a long-range AF order at TN = 24 K accompanied with a cusp-like anomaly in the metallic resistivity. Here, we studied the effect of hydrostatic pressure on its electrical transport properties up to 12.5 GPa by using a cubic anvil cell apparatus. We find that TN determined from the resistivity anomaly first increases slightly with pressure and then decreases until vanished completely at ~7 GPa. Intriguingly, its resistivity rho(T) is enhanced gradually by pressure, and evolves from metallic to activated behavior as the AF order is suppressed. From the Hall resistivity measurements, we confirm that the n-type carriers dominate the transport properties and the carrier density is raised by pressure. In addition, the critical magnetic field Hc1 ~3.3 T at 0 GPa for the spin-flop transition to the canted AF state is found to increase to ~ 5 T and 7.5 T at 1 and 3 GPa. High-pressure XRD evidenced no structural transition up to 12.8 GPa. Based on the Hall resistivity results and first-principles calculations, we proposed that the intralayer direct AF interactions are strengthened by pressure and the competition between AF and FM interactions not only prevents long-range magnetic order but also promotes charge carrier localizations through enhance magnetic fluctuations at high pressures. △ Less

Submitted 3 July, 2019; originally announced July 2019.

Comments: 12 pages, 4 figures

Journal ref: Phys. Rev. Materials 3, 094201 (2019)

Local Superconductivity in Vanadium Iron Arsenide

Authors: Athena S. Sefat, Giang D. Nguyen, David S. Parker, Mingming M. Fu, Qiang Zou, An-Ping Li, Huibo B. Cao, 3 L. Duminda Sanjeewa, Li Li, Z. Gai

Abstract: We investigate the chemical substitution of group 5 into BaFe2As2 (122) iron arsenide, in the effort to understand why Fe-site hole doping of this compound (e.g., using group 5 or 6) does not yield bulk superconductivity. We find an increase in c-lattice parameter of the BaFe2As2 with the substitution of V, Nb, or Ta; the reduction in c predicts the lack of bulk superconductivity [1] that is confi… ▽ More We investigate the chemical substitution of group 5 into BaFe2As2 (122) iron arsenide, in the effort to understand why Fe-site hole doping of this compound (e.g., using group 5 or 6) does not yield bulk superconductivity. We find an increase in c-lattice parameter of the BaFe2As2 with the substitution of V, Nb, or Ta; the reduction in c predicts the lack of bulk superconductivity [1] that is confirmed here through transport and magnetization results. However, our spectroscopy measurements find a coexistence of antiferromagnetic and local superconducting nanoscale regions in V-122, observed for the first time in a transition-metal hole-doped iron arsenide. In BaFe2As2, there is a complex connection between local parameters such as composition and lattice strain, average lattice details, and the emergence of bulk quantum states such as superconductivity and magnetism. [1] L. M. N. Konzen, and A. S. Sefat, J. Phys.: Condens. Matter 29 (2017), 083001. △ Less

Submitted 30 August, 2019; v1 submitted 8 March, 2019; originally announced March 2019.

Comments: 5 figures (including supplemental)

Journal ref: Phys. Rev. B 100, 104525 (2019)

Lattice Disorder Effect on Magnetic Ordering of Iron Arsenides

Authors: Athena S. Sefat, Xiaoping P. Wang, Yaohua Liu, Qiang Zou, Mingming Fu, Zheng Gai, Ganesh Kalaiselvan, Yogesh Vohra, Li Li, David S. Parker

Abstract: This study investigates the changes of magnetic ordering temperature via nano- and mesoscale structural features in an iron arsenide. Although magnetic ground states in quantum materials can be theoretically predicted from known crystal structures and chemical compositions, the ordering temperature is harder to pinpoint due to such local lattice variations. In this work we find surprisingly that a… ▽ More This study investigates the changes of magnetic ordering temperature via nano- and mesoscale structural features in an iron arsenide. Although magnetic ground states in quantum materials can be theoretically predicted from known crystal structures and chemical compositions, the ordering temperature is harder to pinpoint due to such local lattice variations. In this work we find surprisingly that a locally disordered material can exhibit a significantly larger Neel temperature (TN) than an ordered material of precisely the same chemical stoichiometry. Here, a EuFe2As2 crystal, which is a 122 parent of iron arsenide superconductors, is found through synthesis to have ordering below TN = 195 K (for the disordered crystal) or TN = 175 K (for the ordered crystal). In the higher TN crystals, there are shorter planar Fe-Fe bonds [2.7692(2) A vs. 2.7745(3) A], a randomized in-plane defect structure, and diffuse scattering along the [00L] crystallographic direction that manifests as a rather broad specific heat peak. For the lower TN crystals, the a-lattice parameter is larger and the in-plane microscopic structure shows defect ordering along the antiphase boundaries, giving a larger TN and a higher superconducting temperature (Tc) upon the application of pressure. First principles calculations find a strong interaction between c-axis strain and interlayer magnetic coupling, but little impact of planar strain on the magnetic order. Neutron single-crystal diffraction shows that the low-temperature magnetic phase transition due to localized Eu moments is not lattice or disorder sensitive, unlike the higher-temperature Fe sublattice ordering. This study demonstrates a higher magnetic ordering point arising from local disorder in 122. △ Less

Submitted 31 May, 2019; v1 submitted 6 March, 2019; originally announced March 2019.

Comments: 4 main figures

Journal ref: Scientific Reports 9, 20147 (2019)

Inferring Microclimate Zones from Energy Consumption Data

Authors: D. S. Parker, Thuy Vu

Abstract: Climate zones are an established part of urban energy management. California is divided into 16 climate zones, for example, and each zone imposes different energy-related building standards -- so for example different zones have different roofing standards. Although developed long ago, these zones continue to shape urban policy. New climate zone definitions are now emerging in urban settings. Both… ▽ More Climate zones are an established part of urban energy management. California is divided into 16 climate zones, for example, and each zone imposes different energy-related building standards -- so for example different zones have different roofing standards. Although developed long ago, these zones continue to shape urban policy. New climate zone definitions are now emerging in urban settings. Both the County of Los Angeles and the US Department of Energy have recently adopted refined zones -- for restructuring electricity rates, and for scoring home energy efficiency. Defining new zones is difficult, however, because climates depend on variables that are difficult to map. In this paper we show that Los Angeles climate zones can be inferred from energy use data. We have studied residential electricity consumption (EC) patterns in Los Angeles data. This data permits identification of geographical zones whose EC patterns are characteristically different from surrounding regions. These regions have topographic boundaries in Los Angeles consistent with microclimates. Specifically, our key finding is that EC-microclimate zones -- regions in which block groups have similar Electricity Consumption patterns over time -- resemble environmental microclimate zones. Because they conform to microclimates, but are based directly on EC data, these zones can be useful in urban energy management. We also show how microclimates and household electricity consumption in Los Angeles are strongly linked to socioeconomic variables like income and population density. These links permit data-driven development of microclimate zones that support zone-specific modeling and improved energy policy. △ Less

Submitted 16 September, 2018; originally announced September 2018.

Magnetic properties of single crystalline itinerant ferromagnet AlFe2B2

Authors: Tej N. Lamichhane, Li Xiang, Qisheng Lin, Tribhuwan Pandey, David S. Parker, Tae-Hoon Kim, Lin Zhou, Matthew J. Kramer, Sergey L. Bud'ko, Paul C. Canfield

Abstract: Single crystals of AlFe$_{2}$B$_{2}$ have been grown using the self flux growth method and then measured the structural properties, temperature and field dependent magnetization, and temperature dependent electrical resistivity at ambient as well as high pressure. The Curie temperature of AlFe$_{2}$B$_{2}$ is determined to be $274$~K. The measured saturation magnetization and the effective moment… ▽ More Single crystals of AlFe$_{2}$B$_{2}$ have been grown using the self flux growth method and then measured the structural properties, temperature and field dependent magnetization, and temperature dependent electrical resistivity at ambient as well as high pressure. The Curie temperature of AlFe$_{2}$B$_{2}$ is determined to be $274$~K. The measured saturation magnetization and the effective moment for paramagnetic Fe-ion indicate the itinerant nature of the magnetism with a Rhode-Wohlfarth ratio $ \frac{M_{C}}{M_{sat}}\approx 1.14$. Temperature dependent resistivity measurements under hydrostatic pressure shows that transition temperature \textit{T$_C$} is suppressed down to 255 K for $p = 2.24$~GPa pressure with a suppression rate of $\sim -8.9$~K/GPa. The anisotropy fields and magnetocrystalline anisotropy constants are in reasonable agreement with density functional theory calculations. △ Less

Submitted 16 May, 2018; originally announced May 2018.

Comments: 12 pages, 12 figures

Journal ref: Phys. Rev. Materials 2, 084408 (2018)

Borderline Magnetism: How Does Adding Magnesium to Paramagnetic CeCo$_3$ Make a 450 K Ferromagnet with Large Magnetic Anisotropy?

Authors: Tribhuwan Pandey, David S. Parker

Abstract: A recent experimental study (Phys. Rev. Appl. 9, 024023, 2018) on paramagnetic CeCo$_3$ finds that Magnesium alloying induces a ferromagnetic transition with intrinsic properties large enough for permanent magnet applications. Here we explain these surprising results \textit{via} a first principles study of the electronic structure and magnetism of Magnesium-alloyed CeCo$_3$. We find the origin of… ▽ More A recent experimental study (Phys. Rev. Appl. 9, 024023, 2018) on paramagnetic CeCo$_3$ finds that Magnesium alloying induces a ferromagnetic transition with intrinsic properties large enough for permanent magnet applications. Here we explain these surprising results \textit{via} a first principles study of the electronic structure and magnetism of Magnesium-alloyed CeCo$_3$. We find the origin of this Magnesium-induced ferromagnetic transition to be Stoner physics - the substantial increase in the Fermi-level density-of-states $N(E_F)$ with Mg alloying. Our calculations suggest that both Ce and Co atoms are important for generating large magnetic anisotropy suggesting the viability of Co-3$d$, and Ce-4$f$ interaction for the generation of magnetic anisotropy in magnetic materials. These results offer a new route to the discovery of ferromagnetic materials and provide fundamental insight into the magnetic properties of these alloys △ Less

Submitted 14 August, 2018; v1 submitted 19 February, 2018; originally announced February 2018.

Comments: 10 pages, 8 figures

Journal ref: Phys. Rev. Applied 10, 034038 (2018)

Negative thermal expansion and magnetoelastic coupling in the breathing pyrochlore lattice material LiGaCr4S8

Authors: G. Pokharel, A. F. May, D. S. Parker, S. Calder, G. Ehlers, A. Huq, S. A. J. Kimber, H. Suriya Arachchige, L. Poudel, M. A. McGuire, D. Mandrus, A. D. Christianson

Abstract: The physical properties of the spinel LiGaCr4S8 have been studied with neutron diffraction, X-ray diffraction, magnetic susceptibility and heat capacity measurements. The neutron diffraction and synchrotron X-ray diffraction data reveal negative thermal expansion (NTE) below 111(4) K. The magnetic susceptibility deviates from Curie-Weiss behavior with the onset of NTE. At low temperature a broad p… ▽ More The physical properties of the spinel LiGaCr4S8 have been studied with neutron diffraction, X-ray diffraction, magnetic susceptibility and heat capacity measurements. The neutron diffraction and synchrotron X-ray diffraction data reveal negative thermal expansion (NTE) below 111(4) K. The magnetic susceptibility deviates from Curie-Weiss behavior with the onset of NTE. At low temperature a broad peak in the magnetic susceptibility at 10.3(3) K is accompanied by the return of normal thermal expansion. First principles calculations find a strong coupling between the lattice and the simulated magnetic ground state. These results indicate strong magnetoelastic coupling in LiGaCr4S8. △ Less

Submitted 15 April, 2018; v1 submitted 1 February, 2018; originally announced February 2018.

Journal ref: Phys. Rev. B 97, 134117 (2018)

Magnetic order and interactions in ferrimagnetic Mn3Si2Te6

Authors: Andrew F. May, Yaohua Liu, Stuart Calder, David S. Parker, Tribhuwan Pandey, Ercan Cakmak, Huibo Cao, Jiaqiang Yan, Michael A. McGuire

Abstract: The magnetism in Mn$_3$Si$_2$Te$_6$ has been investigated using thermodynamic measurements, first principles calculations, neutron diffraction and diffuse neutron scattering on single crystals. These data confirm that Mn$_3$Si$_2$Te$_6$ is a ferrimagnet below a Curie temperature of $T_C$ approximately 78K. The magnetism is anisotropic, with magnetization and neutron diffraction demonstrating that… ▽ More The magnetism in Mn$_3$Si$_2$Te$_6$ has been investigated using thermodynamic measurements, first principles calculations, neutron diffraction and diffuse neutron scattering on single crystals. These data confirm that Mn$_3$Si$_2$Te$_6$ is a ferrimagnet below a Curie temperature of $T_C$ approximately 78K. The magnetism is anisotropic, with magnetization and neutron diffraction demonstrating that the moments lie within the basal plane of the trigonal structure. The saturation magnetization of approximately 1.6$μ_B$/Mn at 5K originates from the different multiplicities of the two antiferromagnetically-aligned Mn sites. First principles calculations reveal antiferromagnetic exchange for the three nearest Mn-Mn pairs, which leads to a competition between the ferrimagnetic ground state and three other magnetic configurations. The ferrimagnetic state results from the energy associated with the third-nearest neighbor interaction, and thus long-range interactions are essential for the observed behavior. Diffuse magnetic scattering is observed around the 002 Bragg reflection at 120K, which indicates the presence of strong spin correlations well above $T_C$. These are promoted by the competing ground states that result in a relative suppression of $T_C$, and may be associated with a small ferromagnetic component that produces anisotropic magnetism below $\approx$330K. △ Less

Submitted 6 June, 2017; originally announced June 2017.

Comments: Main article plus Supplemental

Journal ref: Physical Review B 95, 174440 (2017)

The meet operation in the imbalance lattice of maximal instantaneous codes: alternative proof of existence

Authors: Stephan Foldes, D. Stott Parker, Sandor Radeleczki

Abstract: An alternative proof is given of the existence of greatest lower bounds in the imbalance order of binary maximal instantaneous codes of a given size. These codes are viewed as maximal antichains of a given size in the infinite binary tree of 0-1 words. The proof proposed makes use of a single balancing operation instead of expansion and contraction as in the original proof of the existence of glb. An alternative proof is given of the existence of greatest lower bounds in the imbalance order of binary maximal instantaneous codes of a given size. These codes are viewed as maximal antichains of a given size in the infinite binary tree of 0-1 words. The proof proposed makes use of a single balancing operation instead of expansion and contraction as in the original proof of the existence of glb. △ Less

Submitted 6 October, 2017; v1 submitted 21 February, 2017; originally announced February 2017.

MSC Class: 06A07; 94A45

Effect of surface morphology and magnetic impurities on the electronic structure in cobalt-doped BaFe2As2 superconductors

Authors: Qiang Zou, Zhiming Wu, Mingming Fu, Chunmiao Zhang, Shivani Rajput, Yaping Wu, Li Li, David S. Parker, Junyong Kang, Athena S. Sefat, Zheng Gai

Abstract: Combined scanning tunneling microscopy, spectroscopy and local barrier height (LBH) studies show that low-temperature-cleaved optimally-doped Ba(Fe1-xCox)2As2 crystals with x=0.06, with Tc = 22 K, have complicated morphologies. Although the cleavage surface and hence the morphologies are variable, the superconducting gap maps show the same gap widths and nanometer size inhomogeneities irrelevant t… ▽ More Combined scanning tunneling microscopy, spectroscopy and local barrier height (LBH) studies show that low-temperature-cleaved optimally-doped Ba(Fe1-xCox)2As2 crystals with x=0.06, with Tc = 22 K, have complicated morphologies. Although the cleavage surface and hence the morphologies are variable, the superconducting gap maps show the same gap widths and nanometer size inhomogeneities irrelevant to the morphology. Based on the spectroscopy and LBH maps, the bright patches and dark stripes in the morphologies are identified as Ba and As dominated surface terminations, respectively. Magnetic impurities, possibly due to cobalt or Fe atoms, are believed to create local in-gap state and in addition suppress the superconducting coherence peaks. This study will clarify the confusion on the cleavage surface terminations of the Fe-based superconductors, and its relation with the electronic structures. △ Less

Submitted 1 February, 2017; originally announced February 2017.

Comments: Accepted to Nano Letters (5 figures)

Discovery of ferromagnetism with large magnetic anisotropy in ZrMnP and HfMnP

Authors: Tej N. Lamichhane, Valentin Taufour, Morgan W. Masters, David S. Parker, Udhara S. Kaluarachchi, Srinivasa Thimmaiah, Sergey L. Bud'ko, Paul C. Canfield

Abstract: ZrMnP and HfMnP single crystals are grown by a self-flux growth technique and structural as well as temperature dependent magnetic and transport properties are studied. Both compounds have an orthorhombic crystal structure. ZrMnP and HfMnP are ferromagnetic with Curie temperatures around $370$~K and $320$~K respectively. The spontaneous magnetizations of ZrMnP and HfMnP are determined to be $1.9$~… ▽ More ZrMnP and HfMnP single crystals are grown by a self-flux growth technique and structural as well as temperature dependent magnetic and transport properties are studied. Both compounds have an orthorhombic crystal structure. ZrMnP and HfMnP are ferromagnetic with Curie temperatures around $370$~K and $320$~K respectively. The spontaneous magnetizations of ZrMnP and HfMnP are determined to be $1.9$~$μ_\textrm{B}$/f.u. and $2.1$~$μ_\textrm{B}$/f.u. respectively at $50$~K. The magnetocaloric effect of ZrMnP in term of entropy change ($ΔS$) is estimated to be $-6.7$ kJm$^{-3}$K$^{-1}$ around $369$~K. The easy axis of magnetization is [100] for both compounds, with a small anisotropy relative to the [010] axis. At $50$~K, the anisotropy field along the [001] axis is $\sim4.6$~T for ZrMnP and $\sim10$~T for HfMnP. Such large magnetic anisotropy is remarkable considering the absence of rare-earth elements in these compounds. The first principle calculation correctly predicts the magnetization and hard axis orientation for both compounds, and predicts the experimental HfMnP anisotropy field within 25 percent. More importantly, our calculations suggest that the large magnetic anisotropy comes primarily from the Mn atoms suggesting that similarly large anisotropies may be found in other 3d transition metal compounds. △ Less

Submitted 8 December, 2016; originally announced December 2016.

Journal ref: Appl. Phys. Lett. 109, 092402 (2016)

Competition of superconductivity with the structural transition in Mo3Sb7

Authors: G. Z. Ye, J. -G. Cheng, J. -Q. Yan, J. P. Sun, K. Matsubayashi, T. Yamauchi, T. Okada, Q. Zhou, D. S. Parker, B. C. Sales, Y. Uwatoko

Abstract: Prior to the superconducting transition at Tc = 2.3 K, Mo3Sb7 undergoes a symmetry-lowering, cubic-to-tetragonal structural transition at Ts = 53 K. We have monitored the pressure dependence of these two transitions by measuring the resistivity of Mo3Sb7 single crystals under various hydrostatic pressures up to 15 GPa. The application of external pressure enhances Tc but suppresses Ts until Pc ~ 1… ▽ More Prior to the superconducting transition at Tc = 2.3 K, Mo3Sb7 undergoes a symmetry-lowering, cubic-to-tetragonal structural transition at Ts = 53 K. We have monitored the pressure dependence of these two transitions by measuring the resistivity of Mo3Sb7 single crystals under various hydrostatic pressures up to 15 GPa. The application of external pressure enhances Tc but suppresses Ts until Pc ~ 10 GPa, above which a pressure-induced first order structural transition takes place and is manifested by the phase coexistence in the pressure range 8 < P < 12 GPa. The cubic phase above 12 GPa is also found to be superconducting with a higher Tc =6 K that decreases slightly with further increasing pressure. The variations with pressure of Tc and Ts satisfy the Bilbro-McMillan equation, i.e. Tc^nTs^(1-n) = constant, thus suggesting the competition of superconductivity with the structural transition that has been proposed to be accompanied with a spin-gap formation at Ts. This scenario is supported by our first-principles calculations which imply the plausible importance of magnetism that competes with the superconductivity in Mo3Sb7. △ Less

Submitted 7 November, 2016; originally announced November 2016.

Comments: 6 figures, Submitted to PRB

Journal ref: Phys. Rev. B 94, 224508 (2016)

Competing magnetic ground states and their coupling to the crystal lattice in CuFe2Ge2

Authors: Andrew F. May, Stuart Calder, David S. Parker, Brian C. Sales, Michael A. McGuire

Abstract: Identifying and characterizing systems with coupled and competing interactions is central to the development of physical models that can accurately describe and predict emergent behavior in condensed matter systems. This work demonstrates that the metallic compound CuFe$_2$Ge$_2$ has competing magnetic ground states, which are shown to be strongly coupled to the lattice and easily manipulated usin… ▽ More Identifying and characterizing systems with coupled and competing interactions is central to the development of physical models that can accurately describe and predict emergent behavior in condensed matter systems. This work demonstrates that the metallic compound CuFe$_2$Ge$_2$ has competing magnetic ground states, which are shown to be strongly coupled to the lattice and easily manipulated using temperature and applied magnetic fields. Temperature-dependent magnetization $M$ measurements reveal a ferromagnetic-like onset at 228(1)\,K and a broad maximum in $M$ near 180\,K. Powder neutron diffraction confirms antiferromagnetic ordering below $T_{\textrm{N}}\approx$175\,K, and an incommensurate spin density wave is observed below $\approx$125\,K. Coupled with the small refined moments (0.5-1\,$μ_B$/Fe), this provides a picture of itinerant magnetism in CuFe$_2$Ge$_2$. The neutron diffraction data also reveal a coexistence of two magnetic phases that further highlights the near-degeneracy of various magnetic states. These results demonstrate that the ground state in CuFe$_2$Ge$_2$ can be easily manipulated by external forces, making it of particular interest for doping, pressure, and further theoretical studies. △ Less

Submitted 18 October, 2016; originally announced October 2016.

Comments: Combines main article and supplemental information

Journal ref: Sci. Rep. 6, 35325 (2016)

Persistent Magnetism in Silver-doped BaFe2As2 Crystals

Authors: Li Li, Huibo Cao, David S. Parker, Stephen J. Kuhn, Athena S. Sefat

Abstract: We investigate the thermodynamic and transport properties of silver-substituted BaFe2As2 (122) crystals, up to ~4.5%. Similar to other transition-metal substitutions in 122, Ag diminishes the antiferromagnetic (TN) and structural (TS) transition temperatures, but unlike other electron-doped 122s, TN and TS coincide without splitting. Although magnetism drops precipitously to TN = 84 K at doping x… ▽ More We investigate the thermodynamic and transport properties of silver-substituted BaFe2As2 (122) crystals, up to ~4.5%. Similar to other transition-metal substitutions in 122, Ag diminishes the antiferromagnetic (TN) and structural (TS) transition temperatures, but unlike other electron-doped 122s, TN and TS coincide without splitting. Although magnetism drops precipitously to TN = 84 K at doping x = 0.029, it only weakly changes above this x, settling at TN = 80 K at x = 0.045. Compared to this persistent magnetism in Ag-122, doping other group 11 elements of either Cu or Au in 122 diminished TN and induced superconductivity near TC = 2 K at x = 0.044 or 0.031, respectively. Ag-122 crystals show reflective surfaces with surprising thicker cross sections for x >= 0.019, the appearance that is in contrast to the typical thin stacked layered feature seen in all other flux-grown x122 and lower Ag-122. This physical trait may be a manifest of intrinsic weak changes in c-lattice and TN. Our theoretical calculations suggest that Ag doping produces strong electronic scattering and yet a relatively small disruption of the magnetic state, both of which preclude superconductivity in this system. △ Less

Submitted 11 July, 2016; originally announced July 2016.

Comments: 13 pages, 7 figures, 1 table

Journal ref: Phys. Rev. B 94, 134510 (2016)

Multi-layered chalcogenides with potential for magnetism and superconductivity

Authors: L. Li, D. S. Parker, C. R. dela Cruz, A. S. Sefat

Abstract: Layered thallium copper chalcogenides can form single, double, or triple layers of Cu-Ch separated by Tl sheets. Here we report on the preparation and properties of Tl-based materials of TlCu2Se2, TlCu4S3, TlCu4Se3 and TlCu6S4, and compare to reports on layered ACu2nChn+1 materials with A = Ba, K, Rb, and Cs, and Ch = S, Se. Having no long-range magnetism for these materials is quite surprising co… ▽ More Layered thallium copper chalcogenides can form single, double, or triple layers of Cu-Ch separated by Tl sheets. Here we report on the preparation and properties of Tl-based materials of TlCu2Se2, TlCu4S3, TlCu4Se3 and TlCu6S4, and compare to reports on layered ACu2nChn+1 materials with A = Ba, K, Rb, and Cs, and Ch = S, Se. Having no long-range magnetism for these materials is quite surprising considering the possibilities of inter- and intra-layer exchange interactions through Cu 3d, and we measure by magnetic susceptibility and confirm by neutron diffraction. First principles density-functional theory calculations for both the single-layer TlCu2Se2 (isostructural to the 122 iron-based superconductors) and the double-layer TlCu4Se3 suggest a lack of Fermi-level spectral weight that is needed to drive a magnetic or superconducting instability. The electronic structure calculations show a much greater likelihood of magnetism for multiple structural layers with Fe. △ Less

Submitted 24 March, 2016; originally announced March 2016.

Comments: 8 pages

Journal ref: Physica C: Superconductivity and its applications 531 (2016), 25

Superconductivity at 9K in Mo5PB2 with evidence for multiple gaps

Authors: Michael A. McGuire, David S. Parker

Abstract: Superconductivity is observed with critical temperatures near 9K in the tetragonal compound Mo5PB2. This material adopts the Cr5B3 structure type common to supercondcuting Nb5Si3-xBx, Mo5SiB2, and W5SiB2, which have critical temperatures of 5.8-7.8 K. We have synthesized polycrystalline samples of the compound, made measurements of electrical resistivity, magnetic susceptibility, and heat capacity… ▽ More Superconductivity is observed with critical temperatures near 9K in the tetragonal compound Mo5PB2. This material adopts the Cr5B3 structure type common to supercondcuting Nb5Si3-xBx, Mo5SiB2, and W5SiB2, which have critical temperatures of 5.8-7.8 K. We have synthesized polycrystalline samples of the compound, made measurements of electrical resistivity, magnetic susceptibility, and heat capacity, and performed first principles electronic structure calculations. The highest Tc value (9.2 K) occurs in slightly phosphorus rich samples, with composition near Mo5P1.1B1.9, and the upper critical field Hc2 at T = 0 is estimated to be about 17 kOe. Together, the measurements and band structure calculations indicate intermediate coupling (lambda = 1.0), phonon mediated superconductivity. The temperature dependence of the heat capacity and upper critical field Hc2 below Tc suggest multiple superconducting gaps may be present. △ Less

Submitted 9 March, 2016; originally announced March 2016.

Journal ref: Physical Review B 93, 064507 (2016)

Extended Magnetic Exchange Interactions in the High-Temperature Ferromagnet MnBi

Authors: T. J. Williams, A. E. Taylor, A. D. Christianson, S. E. Hahn, R. S. Fishman, D. S. Parker, M. A. McGuire, B. C. Sales, M. D. Lumsden

Abstract: The high-temperature ferromagnet MnBi continues to receive attention as a candidate to replace rare-earth-containing permanent magnets in applications above room temperature. This is due to a high Curie temperature, large magnetic moments, and a coercivity that increases with temperature. The synthesis of MnBi also allows for crystals that are free of interstitial Mn, enabling more direct access t… ▽ More The high-temperature ferromagnet MnBi continues to receive attention as a candidate to replace rare-earth-containing permanent magnets in applications above room temperature. This is due to a high Curie temperature, large magnetic moments, and a coercivity that increases with temperature. The synthesis of MnBi also allows for crystals that are free of interstitial Mn, enabling more direct access to the key interactions underlying the physical properties of binary Mn-based ferromagnets. In this work, we use inelastic neutron scattering to measure the spin waves of MnBi in order to characterize the magnetic exchange at low temperature. Consistent with the spin reorientation that occurs below 140 K, we do not observe a spin gap in this system above our experimental resolution. A Heisenberg model was fit to the spin wave data in order to characterize the long-range nature of the exchange. It was found that interactions up to sixth nearest neighbor are required to fully parameterize the spin waves. Surprisingly, the nearest-neighbor term is antiferromagnetic, and the realization of a ferromagnetic ground state relies on the more numerous ferromagnetic terms beyond nearest neighbor, suggesting that the ferromagnetic ground state arises as a consequence of the long-ranged interactions in the system. △ Less

Submitted 10 March, 2016; v1 submitted 8 March, 2016; originally announced March 2016.

Comments: 5 pages, 2 figures, 2 tables; Supplemental Information has 2 pages, 1 figure

Journal ref: Appl. Phys. Lett. 108, 192403 (2016)

FeS: Structure and Composition Relations to Superconductivity and Magnetism

Authors: S. J. Kuhn, M. K. Kidder, W. M. Chance, C. dela Cruz, M. A. McGuire, D. S. Parker, L. Li, L. Debeer-Schmitt, J. Ermentrout, K. Littrell, M. R. Eskildsen, A. S. Sefat

Abstract: Structure and composition of iron chalcogenides have a delicate relationship with magnetism and superconductivity. In this report we investigate the iron sulfide layered tetragonal phase (t-FeS), and compare with three-dimensional hexagonal phase (h-FeS). X-ray diffraction reveals the absence of structural transitions for both t- and h-FeS below room temperature, and gives phase compositions of Fe… ▽ More Structure and composition of iron chalcogenides have a delicate relationship with magnetism and superconductivity. In this report we investigate the iron sulfide layered tetragonal phase (t-FeS), and compare with three-dimensional hexagonal phase (h-FeS). X-ray diffraction reveals the absence of structural transitions for both t- and h-FeS below room temperature, and gives phase compositions of Fe0.93(1)S and Fe0.84(1)S, respectively, for the samples studied here. The a lattice parameter of bigger than 3.68 A is significant for causing bulk superconductivity in iron sulfide, which is controlled by composition and structural details such as iron stoichiometry and concentration of vacancy. While h-FeS with a = 3.4436(1) A has magnetic ordering well above room temperature, our t-FeS with a =3.6779(8)A shows filamentary superconductivity below Tc = 4 K with less than 15% superconducting volume fraction. Also for t-FeS, the magnetic susceptibility shows an anomaly at ~ 15 K, and neutron diffraction reveals a commensurate antiferromagnetic ordering below TN = 116 K, with wave vector km= (0.25,0.25,0) and 0.46(2)uB/Fe. Although two synthesis routes are used here to stabilize t vs h crystal structures (hydrothermal vs solid-state methods), both FeS compounds order on two length-scales of ~1000 nm sheets or blocks and ~ 20 nm smaller particles, shown by neutron scattering. First principles calculations reveal a high sensitivity to the structure for the electronic and magnetic properties in t-FeS, predicting marginal antiferromagnetic instability for our compound (sulfur height of zS ~0.252) with an ordering energy of ~11 meV/Fe, while h-FeS is magnetically stable. △ Less

Submitted 4 March, 2016; originally announced March 2016.

Comments: 14 pages, 7 figures

Journal ref: Physica C: Superconductivity and its applications 534 (2017), 29-36

Anomalous magneto-elastic and charge doping effects in thallium-doped BaFe2As2

Authors: A. S. Sefat, L. Li, H. B. Cao, M. A. McGuire, B. Sales, R. Custelcean, D. S. Parker

Abstract: Within the BaFe2As2 crystal lattice, we partially substitute thallium for barium and report the effects of interlayer coupling in Ba1-xTlxFe2As2 crystals. We demonstrate the unusual effects of magneto-elastic coupling and charge doping in this iron-arsenide material, whereby Neel temperature rises with small x, and then falls with additional x. Specifically, we find that Neel and structural transi… ▽ More Within the BaFe2As2 crystal lattice, we partially substitute thallium for barium and report the effects of interlayer coupling in Ba1-xTlxFe2As2 crystals. We demonstrate the unusual effects of magneto-elastic coupling and charge doping in this iron-arsenide material, whereby Neel temperature rises with small x, and then falls with additional x. Specifically, we find that Neel and structural transitions in BaFe2As2 (TN =Ts= 133 K) increase for x=0.05 (TN = 138 K, Ts = 140 K) from magnetization, heat capacity, resistivity, and neutron diffraction measurements. Evidence from single crystal X-ray diffraction and first principles calculations attributes the stronger magnetism in x=0.05 to magneto-elastic coupling related to the shorter intraplanar Fe-Fe bond distance. With further thallium substitution, the transition temperatures decrease for x = 0.09 (TN = Ts = 131 K), and this is due to charge doping. We illustrate that small changes related to 3d transition-metal state can have profound effects on magnetism. △ Less

Submitted 7 November, 2015; originally announced November 2015.

Comments: 10 pages; 4 figures

Journal ref: Scientific Reports 6 (2016), 21660

Structural and Magnetic Phase Transitions in CeCu$_{6-x}T_x$ ($T$ = Ag, Pd)

Authors: L. Poudel, C. de la Cruz, E. A. Payzant, A. F. May, M. Koehler, V. O. Garlea, A. E. Taylor, D. S. Parker, H. B. Cao, M. A. McGuire, W. Tian, M. Matsuda, H. Jeen, H. N. Lee, T. Hong, S. Calder, H. D. Zhou, M. D. Lumsden, V. Keppens, D. Mandrus, A. D. Christianson

Abstract: The structural and the magnetic properties of CeCu$_{6-x}$Ag$_x$ (0 $\leq$ $x$ $\leq$ 0.85) and CeCu$_{6-x}$Pd$_x$ (0 $\leq$ $x$ $\leq$ 0.4) have been studied using neutron diffraction, resonant ultrasound spectroscopy (RUS), heat capacity, x-ray diffraction measurements and first principles calculations. The structural and magnetic phase diagrams of CeCu$_{6-x}$Ag$_x$ and CeCu$_{6-x}$Pd$_x$ as a… ▽ More The structural and the magnetic properties of CeCu$_{6-x}$Ag$_x$ (0 $\leq$ $x$ $\leq$ 0.85) and CeCu$_{6-x}$Pd$_x$ (0 $\leq$ $x$ $\leq$ 0.4) have been studied using neutron diffraction, resonant ultrasound spectroscopy (RUS), heat capacity, x-ray diffraction measurements and first principles calculations. The structural and magnetic phase diagrams of CeCu$_{6-x}$Ag$_x$ and CeCu$_{6-x}$Pd$_x$ as a function of Ag/Pd composition are reported. The end member, CeCu$_6$, undergoes a structural phase transition from an orthorhombic ($Pnma$) to a monoclinic ($P2_1/c$) phase at 240 K. In CeCu$_{6-x}$Ag$_x$, the structural phase transition temperature (${T_{s}}$) decreases linearly with Ag concentration and extrapolates to zero at $x_{S}$ $\approx$ 0.1. The structural transition in CeCu$_{6-x}$Pd$_x$ remains unperturbed with Pd substitution within the range of our study. The lattice constant $b$ slightly decreases with Ag/Pd doping, whereas, $a$ and $c$ increase with an overall increase in the unit cell volume. Both systems, CeCu$_{6-x}$Ag$_x$ and CeCu$_{6-x}$Pd$_x$, exhibit a magnetic quantum critical point (QCP), at $x$ $\approx$ 0.2 and $x$ $\approx$ 0.05 respectively. Near the QCP, long range antiferromagnetic ordering takes place at an incommensurate wave vector ($δ_1$ 0 $δ_2$) where $δ_1 \sim 0.62$, $δ_2 \sim 0.25$, $x$ = 0.125 for CeCu$_{6-x}$Pd$_x$ and $δ_1 \sim 0.64$, $δ_2 \sim 0.3$, $x$ = 0.3 for CeCu$_{6-x}$Ag$_x$. The magnetic structure consists of an amplitude modulation of the Ce-moments which are aligned along the $c$-axis of the orthorhombic unit cell. △ Less

Submitted 25 November, 2015; v1 submitted 1 October, 2015; originally announced October 2015.

Comments: 13 pages, 9 figures

Journal ref: Phys. Rev. B 92, 214421 (2015)

Magnetic and structural properties of ferromagnetic Fe5PB2 and Fe5SiB2 and effects of Co and Mn substitutions

Authors: Michael A. McGuire, David S. Parker

Abstract: Crystallographic and magnetic properties of Fe5PB2, Fe4CoPB2, Fe4MnPB2, Fe5SiB2, Fe4CoSiB2, and Fe4MnSiB2 are reported. All adopt the tetragonal Cr5B3 structure-type and are ferromagnetic at room temperature with easy axis of magnetization along the c-axis. The spin reorientation in Fe5SiB2 is observed as an anomaly in the magnetization near 170 K, and is suppressed by substitution of Co or Mn for… ▽ More Crystallographic and magnetic properties of Fe5PB2, Fe4CoPB2, Fe4MnPB2, Fe5SiB2, Fe4CoSiB2, and Fe4MnSiB2 are reported. All adopt the tetragonal Cr5B3 structure-type and are ferromagnetic at room temperature with easy axis of magnetization along the c-axis. The spin reorientation in Fe5SiB2 is observed as an anomaly in the magnetization near 170 K, and is suppressed by substitution of Co or Mn for Fe. The silicides are found to generally have larger magnetic moments than the phosphides, but the data suggests smaller magnetic anisotropy in the silicides. Cobalt substitution reduces the Curie temperatures by more than 100 K and ordered magnetic moments by 16-20%, while manganese substitution has a much smaller effect. This suggests Mn moments align ferromagnetically with the Fe and that Co does not have an ordered moment in these structures. Anisotropic thermal expansion is observed in Fe5PB2 and Fe5SiB2, with negative thermal expansion seen along the c-axis of Fe5SiB2. First principles calculations of the magnetic properties of Fe5SiB2 and Fe4MnSiB2 are reported. The results, including the magnetic moment and anisotropy, and are in good agreement with experiment. △ Less

Submitted 8 September, 2015; originally announced September 2015.

Growth and Characterization of Ce- Substituted Nd2Fe14B Single Crystals

Authors: M. A. Susner, B. S. Conner, B. I. Saparov, M. A. McGuire, E. J. Crumlin, G. M. Veith, H. B. Cao, K. V. Shanavas, D. S. Parker, B. C. Chakoumakos, B. C. Sales

Abstract: Single crystals of (Nd1-xCex)2Fe14B are grown out of Fe-(Nd,Ce) flux. Chemical and structural analysis of the crystals indicates that (Nd1-xCex)2Fe14B forms a solid solution until at least x = 0.38 with a Vegard-like variation of the lattice constants with x. Refinements of single crystal neutron diffraction data indicate that Ce has a slight site preference (7:3) for the 4g rare earth site over t… ▽ More Single crystals of (Nd1-xCex)2Fe14B are grown out of Fe-(Nd,Ce) flux. Chemical and structural analysis of the crystals indicates that (Nd1-xCex)2Fe14B forms a solid solution until at least x = 0.38 with a Vegard-like variation of the lattice constants with x. Refinements of single crystal neutron diffraction data indicate that Ce has a slight site preference (7:3) for the 4g rare earth site over the 4f site. Magnetization measurements show that for x = 0.38 the saturation magnetization at 400 K, a temperature important to applications, falls from 29.8 for the parent Nd2Fe14B to 27.6 (mu)B/f.u., the anisotropy field decreases from 5.5 T to 4.7 T, and the Curie temperature decreases from 586 to 543 K. First principles calculations carried out within density functional theory are used to explain the decrease in magnetic properties due to Ce substitution. Though the presence of the lower-cost and more abundant Ce slightly affects these important magnetic characteristics, this decrease is not large enough to affect a multitude of applications. Ce-substituted Nd2Fe14B is therefore a potential high-performance permanent magnet material with substantially reduced Nd content. △ Less

Submitted 31 August, 2015; originally announced August 2015.

Comments: 11 Pages, 8 figures, 5 tables

A study of the physical properties of single crystalline Fe5B2P

Authors: Tej N. Lamichhane, Valentin Taufour, Srinivasa Thimmaiah, David S. Parker, Sergey L. Budko, Paul C. Canfield

Abstract: Single crystals of Fe5B2P were grown by self-flux growth technique. Structural and magnetic properties are studied. The Curie temperature of Fe5B2P is determined to be 655$pm$2K. The saturation magnetization is determined to be 1.72 MuB/Fe at 2K. The temperature variation of the anisotropy constant K1 is determined for the first time, reaching ~0.50 MJ/m3 at 2K, and it is comparable to that of har… ▽ More Single crystals of Fe5B2P were grown by self-flux growth technique. Structural and magnetic properties are studied. The Curie temperature of Fe5B2P is determined to be 655$pm$2K. The saturation magnetization is determined to be 1.72 MuB/Fe at 2K. The temperature variation of the anisotropy constant K1 is determined for the first time, reaching ~0.50 MJ/m3 at 2K, and it is comparable to that of hard ferrites. The saturation magnetization is found to be larger than the hard ferrites. The first principle calculations of saturation magnetization and anisotropy constant are found to be consistent with the experimental results. △ Less

Submitted 23 August, 2015; originally announced August 2015.

Out-of-Plane Spin-Orientation Dependent Magnetotransport Properties in the Anisotropic Helimagnet Cr$_{1/3}$NbS$_2$

Authors: Alexander C. Bornstein, Benjamin J. Chapman, Nirmal J. Ghimire, David G. Mandrus, David S. Parker, Minhyea Lee

Abstract: Understanding the role of spin-orbit coupling (SOC) has been crucial to controlling magnetic anisotropy in magnetic multilayer films. It has been shown that electronic structure can be altered via interface SOC by varying the superlattice structure, resulting in spontaneous magnetization perpendicular or parallel to the plane. In lieu of magnetic thin films, we study the similarly anisotropic heli… ▽ More Understanding the role of spin-orbit coupling (SOC) has been crucial to controlling magnetic anisotropy in magnetic multilayer films. It has been shown that electronic structure can be altered via interface SOC by varying the superlattice structure, resulting in spontaneous magnetization perpendicular or parallel to the plane. In lieu of magnetic thin films, we study the similarly anisotropic helimagnet Cr$_{1/3}$NbS$_2$, where the spin polarization direction, controlled by the applied magnetic field, can modify the electronic structure. As a result, the direction of spin polarization can modulate the density of states, and in turn affect the in-plane electrical conductivity. In Cr$_{1/3}$NbS$_2$, we found an enhancement of in-plane conductivity when the spin polarization is out-of-plane, as compared to in-plane spin polarization. This is consistent with the increase of density of states near the Fermi energy at the same spin configuration, found from first principles calculations. We also observe unusual field dependence of the Hall signal in the same temperature range. This is unlikely to originate from the non-collinear spin texture, but rather further indicates strong dependence of electronic structure on spin orientation relative to the plane. △ Less

Submitted 3 April, 2015; originally announced April 2015.

Comments: 7 pages, 6 figures

Journal ref: Phys. Rev. B 91, 184401 (2015)

Magnetic phase transitions in single crystals of the chiral helimagnet Cr1/3NbS2

Authors: N. J. Ghimire, M. A. McGuire, D. S. Parker, B. Sipos, S. Tang, J. -Q. Yan, B. C. Sales, D. Mandrus

Abstract: The chiral helimagnet Cr1/3NbS2 has been investigated by magnetic, transport and thermal properties measurements on single crystals and by first principles electronic structure calculations. From the measured field and temperature dependence of the magnetization for fields applied perpendicular to the c axis, the magnetic phase diagram has been constructed in the vicinity of the phase transitions.… ▽ More The chiral helimagnet Cr1/3NbS2 has been investigated by magnetic, transport and thermal properties measurements on single crystals and by first principles electronic structure calculations. From the measured field and temperature dependence of the magnetization for fields applied perpendicular to the c axis, the magnetic phase diagram has been constructed in the vicinity of the phase transitions. A transition from a paramagnetic to a magnetically ordered phase occurs near 120 K. With increasing magnetic field and at temperatures below 120 K, this material undergoes transitions from a helimagnetic to a soliton-lattice phase near 900 Oe, and then to a ferromagnetic phase near 1300 Oe. The transitions are found to strongly affect the electrical transport. The resistivity decreases sharply upon cooling near 120 K, and the spin reorientation from the helimagnetic ground state to the commensurate ferromagnetic state is evident in the magnetoresistance. At high fields a large magnetoresistance (55 % at 140 kOe) is observed near the magnetic transition temperature. Heat capacity and electronic structure calculations show the density of states at the Fermi level is low in the magnetically ordered state. Effects of spin fluctuations are likely important in understanding the behavior of Cr1/3NbS2 near and above the magnetic ordering transitions. △ Less

Submitted 13 September, 2012; originally announced September 2012.

Journal ref: Phys. Rev. B 87, 104403 (2013)

Spin reorientation in TlFe1.6Se2 with complete vacancy ordering

Authors: Andrew F. May, Michael A. McGuire, Huibo Cao, Ilya Sergueev, Claudia Cantoni, Bryan C. Chakoumakos, David S. Parker, Brian C. Sales

Abstract: The relationship between vacancy ordering and magnetism in TlFe1.6Se2 has been investigated via single crystal neutron diffraction, nuclear forward scattering, and transmission electron microscopy. The examination of chemically and structurally homogenous crystals allows the true ground state to be revealed, which is characterized by Fe moments lying in the ab-plane below 100K. This is in sharp co… ▽ More The relationship between vacancy ordering and magnetism in TlFe1.6Se2 has been investigated via single crystal neutron diffraction, nuclear forward scattering, and transmission electron microscopy. The examination of chemically and structurally homogenous crystals allows the true ground state to be revealed, which is characterized by Fe moments lying in the ab-plane below 100K. This is in sharp contrast to crystals containing regions of order and disorder, where a competition between c-axis and ab-plane orientations of the moments is observed. The properties of partially-disordered TlFe1.6Se2 are therefore not associated with solely the ordered or disordered regions. This contrasts the viewpoint that phase separation results in independent physical properties in intercalated iron selenides, suggesting a coupling between ordered and disordered regions may play an important role in the superconducting analogues. △ Less

Submitted 12 September, 2012; v1 submitted 5 July, 2012; originally announced July 2012.

Comments: Minor changes; updated references and funding acknowledgement

Journal ref: Phys. Rev. Lett. 109, 077003 (2012)

Complex itinerant ferromagnetism in noncentrosymmetric Cr11Ge19

Authors: N. J. Ghimire, M. A. McGuire, D. S. Parker, B. C. Sales, J. -Q. Yan, V. Keppens, M. Koehler, R. M. Latture, D. Mandrus

Abstract: The noncentrosymmetric ferromagnet Cr11Ge19 has been investigated by electrical transport, AC and DC magnetization, heat capacity, x-ray diffraction, resonant ultrasound spectroscopy, and first principles electronic structure calculations. Complex itinerant ferromagnetism in this material is indicated by nonlinearity in conventional Arrott plots, unusual behavior of AC susceptibility, and a weak h… ▽ More The noncentrosymmetric ferromagnet Cr11Ge19 has been investigated by electrical transport, AC and DC magnetization, heat capacity, x-ray diffraction, resonant ultrasound spectroscopy, and first principles electronic structure calculations. Complex itinerant ferromagnetism in this material is indicated by nonlinearity in conventional Arrott plots, unusual behavior of AC susceptibility, and a weak heat capacity anomaly near the Curie temperature (88 K). The inclusion of spin wave excitations was found to be important in modeling the low temperature heat capacity. The temperature dependence of the elastic moduli and lattice constants, including negative thermal expansion along the c axis at low temperatures, indicate strong magneto-elastic coupling in this system. Calculations show strong evidence for itinerant ferromagnetism and suggest a noncollinear ground state may be expected. △ Less

Submitted 13 June, 2012; v1 submitted 10 April, 2012; originally announced April 2012.

Journal ref: Phys. Rev. B 85, 224405 (2012)