Publications


Multi-band magnetotransport in exfoliated thin films of CuxBi2Se3

Journal of Physics: Condensed Matter, 2018 Institute of Physics Publishing (2018)

JA Alexander-Webber, J Huang, J Beilsten-Edmands, P Cermak, C Drasar, RJ Nicholas, AI Coldea


Implications of bond disorder in a S=1 kagome lattice.

Scientific reports 8 (2018) 4745-4745

JL Manson, J Brambleby, PA Goddard, PM Spurgeon, JA Villa, J Liu, S Ghannadzadeh, F Foronda, J Singleton, T Lancaster, SJ Clark, IO Thomas, F Xiao, RC Williams, FL Pratt, SJ Blundell, CV Topping, C Baines, C Campana, B Noll

Strong hydrogen bonds such as F···H···F offer new strategies to fabricate molecular architectures exhibiting novel structures and properties. Along these lines and, to potentially realize hydrogen-bond mediated superexchange interactions in a frustrated material, we synthesized [H2F]2[Ni3F6(Fpy)12][SbF6]2 (Fpy = 3-fluoropyridine). It was found that positionally-disordered H2F+ ions link neutral NiF2(Fpy)4 moieties into a kagome lattice with perfect 3-fold rotational symmetry. Detailed magnetic investigations combined with density-functional theory (DFT) revealed weak antiferromagnetic interactions (J ~ 0.4 K) and a large positive-D of 8.3 K with ms = 0 lying below ms = ±1. The observed weak magnetic coupling is attributed to bond-disorder of the H2F+ ions which leads to disrupted Ni-F···H-F-H···F-Ni exchange pathways. Despite this result, we argue that networks such as this may be a way forward in designing tunable materials with varying degrees of frustration.


High-Pressure Synthesis, Structures, and Properties of Trivalent A-Site-Ordered Quadruple Perovskites RMn7O12 (R = Sm, Eu, Gd, and Tb).

Inorganic chemistry 57 (2018) 5987-5998

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

A-site-ordered quadruple perovskites RMn7O12 with R = Sm, Eu, Gd, and Tb were synthesized at high pressure and high temperature (6 GPa and ∼1570 K), and their structural, magnetic, and dielectric properties are reported. They crystallize in space group I2/ m at room temperature. All four compounds exhibit a high-temperature phase transition to the cubic Im3̅ structure at ∼664 K (Sm), 663 K (Eu), 657 K (Gd), and 630 K (Tb). They all show one magnetic transition at TN1 ≈ 82-87 K at zero magnetic field, but additional magnetic transitions below TN2 ≈ 12 K were observed in SmMn7O12 and EuMn7O12 at high magnetic fields. Very weak kinklike dielectric anomalies were observed at TN1 in all compounds. We also observed pyroelectric current peaks near 14 K and frequency-dependent sharp steps in dielectric constant (near 18-35 K)-these anomalies are probably caused by dielectric relaxation, and they are not related to any ferroelectric transitions. TbMn7O12 shows signs of nonstoichiometry expressed as (Tb1- xMn x)Mn7O12, and these samples exhibit negative magnetization or magnetization reversal effects of an extrinsic origin on zero-field-cooled curves in intermediate temperature ranges. The crystal structures of SmMn7O12 and EuMn7O12 were refined from neutron powder diffraction data at 100 K, and the crystal structures of GdMn7O12 and (Tb0.88Mn0.12)Mn7O12 were studied by synchrotron X-ray powder diffraction at 295 K.


Coupling between Spin and Charge Order Driven by Magnetic Field in Triangular Ising System LuFe2O4+delta

CRYSTALS 8 (2018) ARTN 88

L Ding, F Orlandi, DD Khalyavin, AT Boothroyd, D Prabhakaran, G Balakrishnan, P Manuel


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.


Ab initio calculation of spin fluctuation spectra using time-dependent density functional perturbation theory, plane waves, and pseudopotentials

PHYSICAL REVIEW B 97 (2018) ARTN 024420

K Cao, H Lambert, PG Radaelli, F Giustino

We present an implementation of time-dependent density functional perturbation theory for spin fluctuations, based on plane waves and pseudopotentials. We compute the dynamic spin susceptibility self-consistently by solving the time-dependent Sternheimer equation, within the adiabatic local density approximation to the exchange and correlation kernel. We demonstrate our implementation by calculating the spin susceptibility of representative elemental transition metals, namely bcc Fe, fcc Ni, and bcc Cr. The calculated magnon dispersion relations of Fe and Ni are in agreement with previous work. The calculated spin susceptibility of Cr exhibits a soft-paramagnon instability, indicating the tendency of the Cr spins to condense in an incommensurate spin density wave phase, in agreement with experiment.


Observation of topological surface states and strong electron/hole imbalance in extreme magnetoresistance compound LaBi

PHYSICAL REVIEW MATERIALS 2 (2018) ARTN 024201

J Jiang, NBM Schroter, S-C Wu, N Kumar, C Shekhar, H Peng, X Xu, C Chen, HF Yang, C-C Hwang, S-K Mo, C Felser, BH Yan, ZK Liu, LX Yang, YL Chen


Electronic Structure and Enhanced Charge-Density Wave Order of Monolayer VSe2.

Nano letters (2018)

J Feng, D Biswas, A Rajan, MD Watson, F Mazzola, OJ Clark, K Underwood, I Marković, M McLaren, A Hunter, DM Burn, LB Duffy, S Barua, G Balakrishnan, F Bertran, P Le Fèvre, TK 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 Na_{1-x}Ca_{x}Mn_{7}O_{12} Quadruple Perovskite Manganites.

Physical review letters 120 (2018) 257202-

RD Johnson, F Mezzadri, P Manuel, DD Khalyavin, E Gilioli, PG Radaelli

We present the discovery and refinement by neutron powder diffraction of a new magnetic phase in the Na_{1-x}Ca_{x}Mn_{7}O_{12} 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.


Microscopic effects of Dy doping in the topological insulator Bi2Te3

PHYSICAL REVIEW B 97 (2018) ARTN 174427

LB Duffy, N-J Steinke, JA Krieger, AI Figueroa, K Kummer, T Lancaster, SR Giblin, FL Pratt, SJ Blundell, T Prokscha, A Suter, S Langridge, VN Strocov, Z Salman, G van der Laan, T Hesjedal


Surface Structure and Reconstructions of HgTe (111) Surfaces

CHINESE PHYSICS LETTERS 35 (2018) ARTN 026802

X-Y Yang, G-Y Wang, C-X Zhao, Z Zhu, L Dong, A-M Li, Y-Y Lv, S-H Yao, Y-B Chen, D-D Guan, Y-Y Li, H Zheng, D Qian, C Liu, Y-L Chen, J-F Jia


Reciprocal space tomography of 3D skyrmion lattice order in a chiral magnet.

Proceedings of the National Academy of Sciences of the United States of America 115 (2018) 6386-6391

S Zhang, G van der Laan, J Müller, L Heinen, M Garst, A Bauer, H Berger, C Pfleiderer, T Hesjedal

It is commonly assumed that surfaces modify the properties of stable materials within the top few atomic layers of a bulk specimen only. Exploiting the polarization dependence of resonant elastic X-ray scattering to go beyond conventional diffraction and imaging techniques, we have determined the depth dependence of the full 3D spin structure of skyrmions-that is, topologically nontrivial whirls of the magnetization-below the surface of a bulk sample of Cu2OSeO3 We found that the skyrmions change exponentially from pure Néel- to pure Bloch-twisting over a distance of several hundred nanometers between the surface and the bulk, respectively. Though qualitatively consistent with theory, the strength of the Néel-twisting at the surface and the length scale of the variation observed experimentally exceed material-specific modeling substantially. In view of the exceptionally complete quantitative theoretical account of the magnetic rigidities and associated static and dynamic properties of skyrmions in Cu2OSeO3 and related materials, we conclude that subtle changes of the materials properties must exist at distances up to several hundred atomic layers into the bulk, which originate in the presence of the surface. This has far-reaching implications for the creation of skyrmions in surface-dominated systems and identifies, more generally, surface-induced gradual variations deep within a bulk material and their impact on tailored functionalities as an unchartered scientific territory.


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

PHYSICAL REVIEW B 97 (2018) ARTN 214422

MC Rahn, J-R Soh, S Francoual, LSI Veiga, J Strempfer, J Mardegan, DY Yan, YF Guo, YG Shi, AT Boothroyd


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

Nature Materials Nature Publishing Group (2018)

FP Chmiel, N Waterfield Price, RD Johnson, AD Lamirand, J Schad, G van der Laan, DT Harris, MS Rzchowski, C-B Eom, PG Radaelli


Proposal for the detection of magnetic monopoles in spin ice via nanoscale magnetometry

PHYSICAL REVIEW B 97 (2018) ARTN 140402

FKK Kirschner, F Flicker, A Yacoby, NY Yao, SJ Blundell


Endohedral Metallofullerene as Molecular High Spin Qubit: Diverse Rabi Cycles in Gd2@C79N.

Journal of the American Chemical Society 140 (2018) 1123-1130

Z Hu, B-W Dong, Z Liu, J-J Liu, J Su, C Yu, J Xiong, D-E Shi, Y Wang, B-W Wang, A Ardavan, Z Shi, S-D Jiang, S Gao

An anisotropic high-spin qubit with long coherence time could scale the quantum system up. It has been proposed that Grover's algorithm can be implemented in such systems. Dimetallic aza[80]fullerenes M2@C79N (M = Y or Gd) possess an unpaired electron located between two metal ions, offering an opportunity to manipulate spin(s) protected in the cage for quantum information processing. Herein, we report the crystallographic determination of Gd2@C79N for the first time. This molecular magnet with a collective high-spin ground state (S = 15/2) generated by strong magnetic coupling (JGd-Rad = 350 ± 20 cm-1) has been unambiguously validated by magnetic susceptibility experiments. Gd2@C79N has quantum coherence and diverse Rabi cycles, allowing arbitrary superposition state manipulation between each adjacent level. The phase memory time reaches 5 μs at 5 K by dynamic decoupling. This molecule fulfills the requirements of Grover's searching algorithm proposed by Leuenberger and Loss.


The key ingredients of the electronic structure of FeSe

Annual Reviews of Condensed Matter Physics, Vol. 9, 125-146, 2018 (2018)

AI Coldea, MD Watson

FeSe is a fascinating superconducting material at the frontier of research in condensed matter physics. Here we provide an overview on the current understanding of the electronic structure of FeSe, focusing in particular on its low energy electronic structure as determined from angular resolved photoemission spectroscopy, quantum oscillations and magnetotransport measurements of single crystal samples. We discuss the unique place of FeSe amongst iron-based superconductors, being a multi-band system exhibiting strong orbitally-dependent electronic correlations and unusually small Fermi surfaces, prone to different electronic instabilities. We pay particular attention to the evolution of the electronic structure which accompanies the tetragonal-orthorhombic structural distortion of the lattice around 90 K, which stabilizes a unique nematic electronic state. Finally, we discuss how the multi-band multi-orbital nematic electronic structure has an impact on the understanding of the superconductivity, and show that the tunability of the nematic state with chemical and physical pressure will help to disentangle the role of different competing interactions relevant for enhancing superconductivity.


Spin dynamics and exchange interactions in CuO measured by neutron scattering

PHYSICAL REVIEW B 97 (2018) ARTN 144401

H Jacobsen, SM Gaw, AJ Princep, E Hamilton, S Toth, RA Ewings, M Enderle, EMH Wheeler, D Prabhakaran, AT Boothroyd


How to probe the spin contribution to momentum relaxation in topological insulators.

Nat Commun 9 (0) 56-

M-S Nam, BH Williams, Y Chen, S Contera, S Yao, M Lu, Y-F Chen, GA Timco, CA Muryn, REP Winpenny, A Ardavan

Topological insulators exhibit a metallic surface state in which the directions of the carriers' momentum and spin are locked together. This characteristic property, which lies at the heart of proposed applications of topological insulators, protects carriers in the surface state from back-scattering unless the scattering centres are time-reversal symmetry breaking (i.e. magnetic). Here, we introduce a method of probing the effect of magnetic scattering by decorating the surface of topological insulators with molecules, whose magnetic degrees of freedom can be engineered independently of their electrostatic structure. We show that this approach allows us to separate the effects of magnetic and non-magnetic scattering in the perturbative limit. We thereby confirm that the low-temperature conductivity of SmB6 is dominated by a surface state and that the momentum of quasiparticles in this state is particularly sensitive to magnetic scatterers, as expected in a topological insulator.


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

Nature communications 9 (2018) 2305-

JM Riley, F Caruso, C Verdi, LB Duffy, MD Watson, 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.

Pages