Publications


Ultra-high critical current densities, the vortex phase diagram and the effect of granularity of the stoichiometric high-Tc superconductor, CaKFe4As4

Physical Review Materials American Physical Society 2 (2018) 074802-

S Singh, M Bristow, WR Meier, P Taylor, S Blundell, PC Canfield, A Coldea

We present a comprehensive study of the critical current densities and the superconducting vortex phase diagram in the stoichiometric superconductor CaKFe4As4 which has a critical temperature of ∼35 K. We performed detailed magnetization measurements both of high quality single crystals for different orientations in an applied magnetic field up to 16 T and for a powder sample. We find an extremely large critical current density, Jc, up to 108 A/cm2 for single crystals when H(ab) at 5 K, which remains robust in fields up to 16 T, being the largest of any other iron-based superconductor. The critical current density is reduced by a factor 10 in single crystals when Hc at 5 K and significantly suppressed by the presence of grain boundaries in the powder sample. We also observe the presence of the fishtail effect in the magnetic hysteresis loops of single crystals when Hc. The flux pinning force density and the pinning parameters suggest that the large critical current could be linked to the existence of point core and surface pinning. Based on the vortex phase diagram and the large critical current densities, CaKFe4As4 is now established as a potential iron-based superconductor candidate for practical applications.


Magnetic X-ray spectroscopy of two-dimensional CrI3 layers

Materials Letters Elsevier 232 (2018) 5-7

A Frisk, LB Duffy, S Zhang, G Van Der Laan, T Hesjedal

The recently confirmed monolayer ferromagnet CrI3 is a frisky example of a two-dimensional ferromagnetic material with great application potential in van der Waals heterostructures. Here we present a soft X-ray absorption spectroscopy study of the magnetic bulk properties of CrI3, giving insight into the magnetic coupling scenario which is relevant for understanding its thickness-dependent magnetic properties. The experimental Cr X-ray magnetic circular dichroism spectra show a good agreement with calculated spectra for a hybridized ground state. In this high-spin Cr ground state the Cr–I bonds show a strongly covalent character. This is responsible for the strong superexchange interaction and increased spin-orbit coupling, resulting in the large magnetic anisotropy of the two-dimensionally layered CrI3 crystal.


Field-induced canting of magnetic moments in GdCo5 at finite temperature: first-principles calculations and high-field measurements

Journal of Physics: Condensed Matter IOP Science 30 (2018) 32LT01

C Patrick, S Kumar, K Götze, MJ Pearce, J Singleton, G Rowlands, G Balakrishnan, Lees, P Goddard, JB Staunton

We present calculations and experimental measurements of the temperature-dependent magnetization of a single crystal of GdCo5 in magnetic fields of order 60 T. At zero temperature the calculations, based on density-functional theory in the disordered-local-moment picture, predict a field-induced transition from an antiferromagnetic to a canted alignment of Gd and Co moments at 46.1 T. At higher temperatures the calculations find this critical field to increase along with the zero-field magnetization. The experimental measurements observe this transition to occur between 44-48 T at 1.4 K. Up to temperatures of at least 100 K, the experiments continue to observe the transition; however, at variance with the calculations, no strong temperature dependence of the critical field is apparent. We assign this difference to the inaccurate description of the zero-field magnetization of the calculations at low temperatures, due to the use of classical statistical mechanics. Correcting for this effect, we recover a consistent description of the high-field magnetization of GdCo5 from theory and experiment.


Magneto-orbital texture in the perovskite modification of Mn2O3

PHYSICAL REVIEW B 98 (2018) ARTN 014426

DD Khalyavin, RD Johnson, P Manuel, AA Tsirlin, AM Abakumov, DP Kozlenko, Y Sun, L Dubrovinsky, SV Ovsyannikov


Maximising the resolving power of the scanning tunneling microscope

Advanced Structural and Chemical Imaging SpringerOpen 4 (2018) 7-

L Jones, S Wang, X Hu, S ur Rahman, M Castell

The usual way to present images from a scanning tunneling microscope (STM) is to take multiple images of the same area, to then manually select the one that appears to be of the highest quality, and then to discard the other almost identical images. This is in contrast to most other disciplines where the signal to noise ratio (SNR) of a data set is improved by taking repeated measurements and averaging them. Data averaging can be routinely performed for 1D spectra, where their alignment is straightforward. However, for serial-acquired 2D STM images the nature and variety of image distortions can severely complicate accurate registration. Here, we demonstrate how a significant improvement in the resolving power of the STM can be achieved through automated distortion correction and multi-frame averaging (MFA) and we demonstrate the broad utility of this approach with three examples. First, we show a sixfold enhancement of the SNR of the Si(111)-(7 × 7) reconstruction. Next, we demonstrate that images with sub-picometre height precision can be routinely obtained and show this for a monolayer of Ti2O3 on Au(111). Last, we demonstrate the automated classification of the two chiral variants of the surface unit cells of the (4 × 4) reconstructed SrTiO3(111) surface. Our new approach to STM imaging will allow a wealth of structural and electronic information from surfaces to be extracted that was previously buried in noise.


Observation of magnetic vortex pairs at room temperature in a planar α-Fe2O3/Co heterostructure

Bulletin of the American Physical Society American Physical Society (2018)

F Chmiel, N Price, R Johnson, A Lamirand, J Schad, GVD Laan, DT Harris, J Irwin, C-B Eom, P Radaelli

Vortices are among the simplest topological structures, and occur whenever a flow field `whirls' around a one-dimensional core. They are ubiquitous to many branches of physics, from fluid dynamics to superconductivity and superfluidity, and are even predicted by some unified theories of particle interactions, where they might explain some of the largest-scale structures seen in today's Universe. In the crystalline state, vortex formation is rare, since it is generally hampered by long-range interactions: in ferroic materials (ferromagnetic and ferroelectric), vortices are only observed when the effects of the dipole-dipole interaction is modified by confinement at the nanoscale, or when the parameter associated with the vorticity does not couple directly with strain. Here, we present the discovery of a novel form of vortices in antiferromagnetic (AFM) hematite ($\alpha$-Fe$_2$O$_3$) epitaxial films, in which the primary whirling parameter is the staggered magnetisation. Remarkably, ferromagnetic (FM) topological objects with the same vorticity and winding number of the $\alpha$-Fe$_2$O$_3$ vortices are imprinted onto an ultra-thin Co ferromagnetic over-layer by interfacial exchange. Our data suggest that the ferromagnetic vortices may be merons (half-skyrmions, carrying an out-of-plane core magnetisation), and indicate that the vortex/meron pairs can be manipulated by the application of an in-plane magnetic field, H$_{\parallel}$, giving rise to large-scale vortex-antivortex annihilation.


THz carrier dynamics and magnetotransport study of topological surface states in thin film Bi<inf>2</inf>Se<inf>3</inf>

Proceedings of SPIE - The International Society for Optical Engineering 10531 (2018)

VS Kamboj, A Singh, T Ferrus, HE Beere, LB Duffy, T Hesjedal, CHW Barnes, DA Ritchie

© 2018 SPIE. The surface of a topological insulator harbors exotic topological states, protected against backscattering from disorder by time reversal symmetry. The study of these exotic quantum states not only provides an opportunity to explore fundamental phenomena in condensed matter physics, such as the spin Hall effect, but also lays the foundation for applications from quantum computing to spintronics. Conventional electrical measurements suffer from substantial bulk interference, making it difficult to clearly distinguish topological surface states from bulk states. Employing terahertz time-domain spectroscopy, we study the temperature-dependent optical behavior of a 23-quintuple-thick film of bismuth selenide (Bi2Se3) allowing for the deconvolution of the surface state response from the bulk. Our measurement of carrier dynamics give an optical mobility exceeding 2100 cm2/V•s at 4 K, indicative of a surface-dominated response, and a scattering lifetime of ∼0.18 ps and a carrier density of 6×1012cm-2at 4 K for the Bi2Se3film. The sample was further processed into a Hall bar device using two different etching techniques, a wet chemical etching and Ar+ion milling, which resulting in a reduced Hall mobility. Even so, the magneto-conductance transport reveals weak antilocalization behavior in our Bi2Se3 sample, consistent with the presence of a single topological surface state mode.


Electronic structure and enhanced charge-density wave order of monolayer VSe2

Nano Letters American Chemical Society 18 (2018) 4493–4499-

J Feng, D Biswas, A Rajan, F Mazzola, OJ Clark, K Underwood, I Marckovic, M McLaren, A Hunter, DM Burn, L Duffy, S Barua, G Balakrishnan, F Bertran, P LeFevre, T Kim, G van der Laan, T Hesjedal, P Wahl, PDC King

How the interacting electronic states and phases of layered transition-metal dichalcogenides evolve when thinned to the single-layer limit is a key open question in the study of two-dimensional materials. Here, we use angle-resolved photoemission to investigate the electronic structure of monolayer VSe2 grown on bilayer graphene/SiC. While the global electronic structure is similar to that of bulk VSe2, we show that, for the monolayer, pronounced energy gaps develop over the entire Fermi surface with decreasing temperature below Tc = 140 ± 5 K, concomitant with the emergence of charge-order superstructures evident in low-energy electron diffraction. These observations point to a charge-density wave instability in the monolayer that is strongly enhanced over that of the bulk. Moreover, our measurements of both the electronic structure and of X-ray magnetic circular dichroism reveal no signatures of a ferromagnetic ordering, in contrast to the results of a recent experimental study as well as expectations from density functional theory. Our study thus points to a delicate balance that can be realized between competing interacting states and phases in monolayer transition-metal dichalcogenides.


Evolution of magneto-orbital order upon B-site electron doping in Na1−xCaxMn7O12 quadruple perovskite manganites

Physical Review Letters American Physical Society 120 (2018) 257202-

R Johnson, F Mezzadri, P Manuel, DD Khalyavin, E Gilioli, PGR Radaelli

We present the discovery and refinement by neutron powder diffraction of a new magnetic phase in the Na1-xCaxMn7O12 quadruple perovskite phase diagram, which is the incommensurate analogue of the well-known pseudo-CE phase of the simple perovskite manganites. We demonstrate that incommensurate magnetic order arises in quadruple perovskites due to the exchange interactions between A and B sites. Furthermore, by constructing a simple mean field Heisenberg exchange model that generically describes both simple and quadruple perovskite systems, we show that this new magnetic phase unifies a picture of the interplay between charge, magnetic and orbital ordering across a wide range of compounds.


Spin-induced multiferroicity in the binary perovskite manganite Mn2O3

Nature Communications Nature Publishing Group 9 (2018) 2996-

J Cong, K Zhai, Y Chai, D Shang, DD Khalyavin, R Johnson, DP Kozlenko, Kichanov, AM Abakumov, AA Tsirlin, L Dubrovinsky, X Xu, Z Sheng, SV Ovsyannikov, Y Sun

The ABO3 perovskite oxides exhibit a wide range of interesting physical phenomena remaining in the focus of extensive scientific investigations and various industrial applications. In order to form a perovskite structure, the cations occupying the A and B positions in the lattice, as a rule, should be different. Nevertheless, the unique binary perovskite manganite Mn2O3 containing the same element in both A and B positions can be synthesized under high-pressure high-temperature conditions. Here, we show that this material exhibits magnetically driven ferroelectricity and a pronounced magnetoelectric effect at low temperatures. Neutron powder diffraction revealed two intricate antiferromagnetic structures below 100 K, driven by a strong interplay between spin, charge, and orbital degrees of freedom. The peculiar multiferroicity in the Mn2O3 perovskite is ascribed to a combined effect involving several mechanisms. Our work demonstrates the potential of binary perovskite oxides for creating materials with highly promising electric and magnetic properties.


Effect of annealing on the structure and magnetic properties of Co2FeAl0.5Si0.5 thin films on Ge(111)

JOURNAL OF ALLOYS AND COMPOUNDS 748 (2018) 323-327

B Kuerbanjiang, C Love, D Kepaptsoglou, Z Nedelkoski, S Yamada, A Ghasemi, QM Ramasse, K Hamaya, SA Cavill, VK Lazarov


Coupling of magnetic order and charge transport in the candidate Dirac semimetal EuCd2As2

Physical review B: Condensed matter and materials physics American Physical Society 97 (2018) 214422

MC Rahn, JR Soh, S Francoual, LSI Veiga, J Strempfer, J Mardegan, DY Yan, YF Guo, YG Shi, A Boothroyd

We use resonant elastic x-ray scattering to determine the evolution of magnetic order in EuCd 2 As 2 below T N = 9.5 K, as a function of temperature and applied magnetic field. We find an A-type antiferromagnetic structure with in-plane magnetic moments, and observe dramatic magnetoresistive effects associated with field-induced changes in the magnetic structure and domain populations. Our ab initio electronic structure calculations indicate that the Dirac dispersion found in the nonmagnetic Dirac semimetal Cd 3 As 2 is also present in EuCd 2 As 2 , but is gapped for T &lt; T N due to the breaking of C 3 symmetry by the magnetic structure.


Doped Sr2FeIrO6-Phase Separation and a Jeff ≠ 0 State for Ir5.

Inorganic chemistry 57 (2018) 10303-10311

JE Page, CV Topping, A Scrimshire, PA Bingham, SJ Blundell, MA Hayward

High-resolution synchrotron X-ray and neutron powder diffraction data demonstrate that, in contrast to recent reports, Sr2FeIrO6 adopts an I1̅ symmetry double perovskite structure with an a-b-c- tilting distortion. This distorted structure does not tolerate cation substitution, with low levels of A-site (Ca, Ba, La) or Fe-site (Ga) substitution leading to separation into two phases: a stoichiometric I1̅ phase and a cation-substituted, P21/ n symmetry, a-a-c+ distorted double perovskite phase. Magnetization, neutron diffraction, and 57Fe Mössbauer data show that, in common with Sr2FeIrO6, the cation substituted Sr2- xA xFe1- yGa yIrO6 phases undergo transitions to type-II antiferromagnetically ordered states at TN ∼ 120 K. However, in contrast to stoichiometric Sr2FeIrO6, cation substituted samples exhibit a further magnetic transition at TA ∼ 220 K, which corresponds to the ordering of Jeff ≠ 0 Ir5+ centers in the cation-substituted, P21/ n symmetry, double perovskite phases.


Preparation and characterization of manganese, cobalt and zinc DNA nanoflowers with tuneable morphology, DNA content and size

Nucleic Acids Research Oxford University Press 2018 (2018)

YR Baker, J Chen, J Brown, AH El-Sagheer, P Wiseman, E Johnson, P Goddard, T Brown

Recently reported DNA nanoflowers are an interesting class of organic-inorganic hybrid materials which are prepared using DNA polymerases. DNA nanoflowers combine the high surface area and scaffolding of inorganic Mg2P2O7 nanocrystals with the targeting properties of DNA, whilst adding enzymatic stability and enhanced cellular uptake. We have investigated conditions for chemically modifying the inorganic core of these nanoflowers through substitution of Mg2+ with Mn2+, Co2+ or Zn2+ and have characterized the resulting particles. These have a range of novel nanoarchitectures, retain the enzymatic stability of their magnesium counterparts and the Co2+ and Mn2+ DNA nanoflowers have added magnetic properties. We investigate conditions to control different morphologies, DNA content, hybridization properties, and size. Additionally, we show that DNA nanoflower production is not limited to Ф29 DNA polymerase and that the choice of polymerase can influence the DNA length within the constructs. We anticipate that the added control of structure, size and chemistry will enhance future applications.


Observation of magnetic vortex pairs at room temperature in a planar α-Fe2O3/Co heterostructure

Nature Materials Nature Publishing Group 17 (2018) 581–585-

F Chmiel, N Waterfield Price, R Johnson, AD Lamirand, J Schad, G van der Laan, DT Harris, C-B Eom, P Radaelli

Vortices, occurring whenever a flow field ‘whirls’ around a one-dimensional core, are among the simplest topological structures, ubiquitous to many branches of physics. In the crystalline state, vortex formation is rare, since it is generally hampered by long-range interactions: in ferroic materials (ferromagnetic and ferroelectric), vortices are observed only when the effects of the dipole–dipole interaction are modified by confinement at the nanoscale1,2,3, or when the parameter associated with the vorticity does not couple directly with strain4. Here, we observe an unprecedented form of vortices in antiferromagnetic haematite (α-Fe2O3) epitaxial films, in which the primary whirling parameter is the staggered magnetization. Remarkably, ferromagnetic topological objects with the same vorticity and winding number as the α-Fe2O3 vortices are imprinted onto an ultra-thin Co ferromagnetic over-layer by interfacial exchange. Our data suggest that the ferromagnetic vortices may be merons (half-skyrmions, carrying an out-of plane core magnetization), and indicate that the vortex/meron pairs can be manipulated by the application of an in-plane magnetic field, giving rise to large-scale vortex–antivortex annihilation.


Persistence of antiferromagnetic order upon La substitution in the 4d4 Mott insulator Ca2RuO4

Physical Review B American Physical Society 98 (2018)

A Boothroyd, D Pincini, S Boseggia, R Perry, M Guttmann, S Ricco, L Veiga, C Dashwood, S Collins, G Nisbet, A Bombardi, D Porter, F Baumberger, D McMorrow

The chemical and magnetic structures of the series of compounds Ca2−xLaxRuO4 [x = 0, 0.05(1), 0.07(1), 0.12(1)] have been investigated using neutron diffraction and resonant elastic x-ray scattering. Upon La doping, the low-temperature S-P bca space group of the parent compound is retained in all insulating samples [x 0.07(1)], but with significant changes to the atomic positions within the unit cell. These changes can be characterized in terms of the local RuO6 octahedral coordination: with increasing doping, the structure, crudely speaking, evolves from an orthorhombic unit cell with compressed octahedra to a quasitetragonal unit cell with elongated ones. The magnetic structure on the other hand, is found to be robust, with the basic k = (0,0,0), b-axis antiferromagnetic order of the parent compound preserved below the critical La doping concentration of x ≈ 0.11. The only effects of La doping on the magnetic structure are to suppress the A-centred mode, favoring the B mode instead, and to reduce the Néel temperature somewhat. Our results are discussed with reference to previous experimental reports on the effects of cation substitution on the d4 Mott insulator Ca2RuO4, as well as with regard to theoretical studies on the evolution of its electronic and magnetic structure. In particular, our results rule out the presence of a proposed ferromagnetic phase, and suggest that the structural effects associated with La substitution play an important role in the physics of the system.


Intrinsic Triple Order in A-site Columnar-Ordered Quadruple Perovskites: Proof of Concept.

Chemphyschem : a European journal of chemical physics and physical chemistry (2018)

AA Belik, DD Khalyavin, L Zhang, Y Matsushita, Y Katsuya, M Tanaka, RD Johnson, K Yamaura

There is an emerging topic in the science of perovskite materials: A-site columnar-ordered A2 A'A''B4 O12 quadruple perovskites, which have an intrinsic triple order at the A sites. However, in many examples reported so far, A' and A'' cations are the same, and the intrinsic triple order is hidden. Here, we investigate structural properties of Dy2 CuMnMn4 O12 (1) and Ho2 MnGaMn4 O12 (2) by neutron and X-ray powder diffraction and prove the triple order at the A sites. The cation distributions determined are [Ho2 ]A [Mn]A' [Ga0.66 Mn0.34 ]A'' [Mn3.66 Ga0.34 ]B O12 and [Dy2 ]A [Cu0.73 Mn0.27 ]A' [Mn0.80 Dy0.20 ]A'' [Mn1.89 Cu0.11 ]B1 [Mn2 ]B2 O12 . There are clear signatures of Jahn-Teller distortions in 1 and 2, and the orbital pattern is combined with an original type of charge ordering in 1. Columnar-ordered quadruple perovskites represent a new playground to study complex interactions between different electronic degrees of freedom. No long-range magnetic order was found in 2 by neutron diffraction, and its magnetic properties in low fields are dominated by an impurity with negative magnetization or magnetization reversal. On the other hand, 1 shows three magnetic transitions at 21, 125, and 160 K.


Pauling entropy, metastability, and equilibrium in Dy2Ti2O7 spin ice

Physical Review Letters American Physical Society 121 (2018) 067202

Giblin, M Twengström, L Bovo, M Ruminy, M Bartkowiak, P Manuel, JC Andresen, D Prabhakaran, G Balakrishnan, E Pomjakushina, C Paulsen, E Lhotel, L Keller, M Frontzek, SC Capelli, O Zaharko, PA McClarty, ST Bramwell, P Henelius, T Fennell

<p>Determining the fate of the Pauling entropy in the classical spin ice material Dy<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub> with respect to the third law of thermodynamics has become an important test case for understanding the existence and stability of ice-rule states in general. The standard model of spin ice—the dipolar spin ice model—predicts an ordering transition at T≈0.15  K, but recent experiments by Pomaranski <em>et al.</em> suggest an entropy recovery over long timescales at temperatures as high as 0.5 K, much too high to be compatible with the theory. Using neutron scattering and specific heat measurements at low temperatures and with long timescales (0.35  K/10<sup>6</sup>  s and 0.5  K/10<sup>5</sup>  s, respectively) on several isotopically enriched samples, we find no evidence of a reduction of ice-rule correlations or spin entropy. High-resolution simulations of the neutron structure factor show that the spin correlations remain well described by the dipolar spin ice model at all temperatures. Furthermore, by careful consideration of hyperfine contributions, we conclude that the original entropy measurements of Ramirez <em>et al.</em> are, after all, essentially correct: The short-time relaxation method used in that study gives a reasonably accurate estimate of the equilibrium spin ice entropy due to a cancellation of contributions.</p>


Crossover from lattice to plasmonic polarons of a spin-polarised electron gas in ferromagnetic EuO

Nature Communications Springer Nature 9 (2018) 2305

JM Riley, F Caruso, C Verdi, LB Duffy, L Bawden, K Volckaert, G van der Laan, T Hesjedal, M Hoesch, F Giustino, PDC King

Strong many-body interactions in solids yield a host of fascinating and potentially useful physical properties. Here, from angle-resolved photoemission experiments and ab initio many-body calculations, we demonstrate how a strong coupling of conduction electrons with collective plasmon excitations of their own Fermi sea leads to the formation of plasmonic polarons in the doped ferromagnetic semiconductor EuO. We observe how these exhibit a significant tunability with charge carrier doping, leading to a polaronic liquid that is qualitatively distinct from its more conventional lattice-dominated analogue. Our study thus suggests powerful opportunities for tailoring quantum many-body interactions in solids via dilute charge carrier doping.


Disentangling orbital and spin exchange interactions for Co2+ on a rocksalt lattice

Physical Review B American Physical Society 98 (2018) 024415

PM Sarte, RA Cowley, EE Rodriguez, E Pachoud, D Le, V García-Sakai, JW Taylor, CD Frost, D Prabhakaran, C Macewen, A Kitada, AJ Browne, M Songvilay, Z Yamani, WJL Buyers, JP Attfield, C Stock

Neutron spectroscopy was applied to study the magnetic interactions of orbitally degenerate Co2+ on a host MgO rocksalt lattice where no long-range spin or orbital order exists. The paramagnetic nature of the substituted monoxide Co0.03Mg0.97O allows for the disentanglement of spin exchange and spin-orbit interactions. By considering the prevalent excitations from Co2+ spin pairs, we extract seven exchange constants out to the fourth coordination shell. An antiferromagnetic next-nearest-neighbor 180◦ exchange interaction is dominant; however, dual ferromagnetic and antiferromagnetic interactions are observed for pairings with other pathways. These interactions can be understood in terms of a combination of orbital degeneracy in the t2g channel and the Goodenough-Kanamori-Anderson rules. Our work suggest that such a hierarchy of exchange interactions exists in transition-metal-based oxides with a t2g orbital degeneracy.

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