Coupled commensurate charge density wave and lattice distortion in Na(2)Ti(2)Pn(2)O (Pn = As,Sb) determined by x-ray diffraction and angle-resolved photoemission spectroscopy

PHYSICAL REVIEW B 94 (2016) ARTN 104515

NR Davies, RD Johnson, AJ Princep, LA Gannon, J-Z Ma, T Qian, P Richard, H Li, M Shi, H Nowell, PJ Baker, YG Shi, H Ding, J Luo, YF Guo, AT Boothroyd

Spin resonance in the superconducting state of Li1-xFexODFe1-ySe observed by neutron spectroscopy

PHYSICAL REVIEW B 94 (2016) ARTN 144503

NR Davies, MC Rahn, HC Walker, RA Ewings, DN Woodruff, SJ Clarke, AT Boothroyd

Atomic-level structural and chemical analysis of Cr-doped Bi2Se3 thin films.

Scientific reports 6 (2016) 26549-

A Ghasemi, D Kepaptsoglou, LJ Collins-McIntyre, Q Ramasse, T Hesjedal, VK Lazarov

We present a study of the structure and chemical composition of the Cr-doped 3D topological insulator Bi2Se3. Single-crystalline thin films were grown by molecular beam epitaxy on Al2O3 (0001), and their structural and chemical properties determined on an atomic level by aberration-corrected scanning transmission electron microscopy and electron energy loss spectroscopy. A regular quintuple layer stacking of the Bi2Se3 film is found, with the exception of the first several atomic layers in the initial growth. The spectroscopy data gives direct evidence that Cr is preferentially substituting for Bi in the Bi2Se3 host. We also show that Cr has a tendency to segregate at internal grain boundaries of the Bi2Se3 film.

Modulated spin helicity stabilized by incommensurate orbital density waves in a quadruple perovskite manganite

PHYSICAL REVIEW B 93 (2016) ARTN 180403

RD Johnson, DD Khalyavin, P Manuel, A Bombardi, C Martin, LC Chapon, PG Radaelli

Evidence for unidirectional nematic bond ordering in FeSe

Physical Review B - Condensed Matter and Materials Physics American Physical Society (2016)

MD Watson, TK Kim, LC Rhodes, M Eschrig, M Hoesch, AA Haghighirad, AI Coldea

The lifting of $d_{xz}$-$d_{yz}$ orbital degeneracy is often considered a hallmark of the nematic phase of Fe-based superconductors, including FeSe, but its origin is not yet understood. Here we report a high resolution Angle-Resolved Photoemission Spectroscopy study of single crystals of FeSe, accounting for the photon-energy dependence and making a detailed analysis of the temperature dependence. We find that the hole pocket undergoes a fourfold-symmetry-breaking distortion in the nematic phase below 90~K, but in contrast the changes to the electron pockets do not require fourfold symmetry-breaking. Instead, there is an additional separation of the existing $d_{xy}$ and $d_{xz/yz}$ bands - which themselves are not split within resolution. These observations lead us to propose a new scenario of "unidirectional nematic bond ordering" to describe the low-temperature electronic structure of FeSe, supported by a good agreement with 10-orbital tight binding model calculations.

Unconventional Superconductivity in the Layered Iron Germanide YFe(2)Ge(2).

Physical review letters 116 (2016) 127001-

J Chen, K Semeniuk, Z Feng, P Reiss, P Brown, Y Zou, PW Logg, GI Lampronti, FM Grosche

The iron-based intermetallic YFe_{2}Ge_{2} stands out among transition metal compounds for its high Sommerfeld coefficient of the order of 100  mJ/(mol K^{2}), which signals strong electronic correlations. A new generation of high quality samples of YFe_{2}Ge_{2} show superconducting transition anomalies below 1.8 K in thermodynamic, magnetic, and transport measurements, establishing that superconductivity is intrinsic in this layered iron compound outside the known superconducting iron pnictide or chalcogenide families. The Fermi surface geometry of YFe_{2}Ge_{2} resembles that of KFe_{2}As_{2} in the high pressure collapsed tetragonal phase, in which superconductivity at temperatures as high as 10 K has recently been reported, suggesting an underlying connection between the two systems.

Coherent Magnetoelastic Domains in Multiferroic BiFeO_{3} Films.

Physical review letters 117 (2016) 177601-

N Waterfield Price, RD Johnson, W Saenrang, F Maccherozzi, SS Dhesi, A Bombardi, FP Chmiel, C-B Eom, PG Radaelli

The physical properties of epitaxial films can fundamentally differ from those of bulk single crystals even above the critical thickness. By a combination of nonresonant x-ray magnetic scattering, neutron diffraction and vector-mapped x-ray magnetic linear dichroism photoemission electron microscopy, we show that epitaxial (111)-BiFeO_{3} films support submicron antiferromagnetic domains, which are magnetoelastically coupled to a coherent crystallographic monoclinic twin structure. This unique texture, which is absent in bulk single crystals, should enable control of magnetism in BiFeO_{3} film devices via epitaxial strain.

Evolution of the Valley Position in Bulk Transition-Metal Chalcogenides and Their Monolayer Limit.

Nano letters 16 (2016) 4738-4745

H Yuan, Z Liu, G Xu, B Zhou, S Wu, D Dumcenco, K Yan, Y Zhang, S-K Mo, P Dudin, V Kandyba, M Yablonskikh, A Barinov, Z Shen, S Zhang, Y Huang, X Xu, Z Hussain, HY Hwang, Y Cui, Y Chen

Layered transition metal chalcogenides with large spin orbit coupling have recently sparked much interest due to their potential applications for electronic, optoelectronic, spintronics, and valleytronics. However, most current understanding of the electronic structure near band valleys in momentum space is based on either theoretical investigations or optical measurements, leaving the detailed band structure elusive. For example, the exact position of the conduction band valley of bulk MoS2 remains controversial. Here, using angle-resolved photoemission spectroscopy with submicron spatial resolution (micro-ARPES), we systematically imaged the conduction/valence band structure evolution across representative chalcogenides MoS2, WS2, and WSe2, as well as the thickness dependent electronic structure from bulk to the monolayer limit. These results establish a solid basis to understand the underlying valley physics of these materials, and also provide a link between chalcogenide electronic band structure and their physical properties for potential valleytronics applications.

Robustness of superconductivity to competing magnetic phases in tetragonal FeS

PHYSICAL REVIEW B 94 (2016) ARTN 134509

FKK Kirschner, F Lang, CV Topping, PJ Baker, FL Pratt, SE Wright, DN Woodruff, SJ Clarke, SJ Blundell

All-in-all-Out Magnetic Order and Propagating Spin Waves in Sm_{2}Ir_{2}O_{7}.

Physical review letters 117 (2016) 037201-

C Donnerer, MC Rahn, MM Sala, JG Vale, D Pincini, J Strempfer, M Krisch, D Prabhakaran, AT Boothroyd, DF McMorrow

Using resonant magnetic x-ray scattering we address the unresolved nature of the magnetic ground state and the low-energy effective Hamiltonian of Sm_{2}Ir_{2}O_{7}, a prototypical pyrochlore iridate with a finite temperature metal-insulator transition. Through a combination of elastic and inelastic measurements, we show that the magnetic ground state is an all-in-all-out (AIAO) antiferromagnet. The magnon dispersion indicates significant electronic correlations and can be well described by a minimal Hamiltonian that includes Heisenberg exchange [J=27.3(6)  meV] and Dzyaloshinskii-Moriya interactions [D=4.9(3)  meV], which provides a consistent description of the magnetic order and excitations. In establishing that Sm_{2}Ir_{2}O_{7} has the requisite inversion symmetry preserving AIAO magnetic ground state, our results support the notion that pyrochlore iridates may host correlated Weyl semimetals.

Ab initio cycloidal and chiral magnetoelectric responses in Cr2O3

PHYSICAL REVIEW B 94 (2016) ARTN 100405

N Tillack, JR Yates, PG Radaelli

Photonic topological insulator with broken time-reversal symmetry.

Proceedings of the National Academy of Sciences of the United States of America 113 (2016) 4924-4928

C He, X-C Sun, X-P Liu, M-H Lu, Y Chen, L Feng, Y-F Chen

A topological insulator is a material with an insulating interior but time-reversal symmetry-protected conducting edge states. Since its prediction and discovery almost a decade ago, such a symmetry-protected topological phase has been explored beyond electronic systems in the realm of photonics. Electrons are spin-1/2 particles, whereas photons are spin-1 particles. The distinct spin difference between these two kinds of particles means that their corresponding symmetry is fundamentally different. It is well understood that an electronic topological insulator is protected by the electron's spin-1/2 (fermionic) time-reversal symmetry [Formula: see text] However, the same protection does not exist under normal circumstances for a photonic topological insulator, due to photon's spin-1 (bosonic) time-reversal symmetry [Formula: see text] In this work, we report a design of photonic topological insulator using the Tellegen magnetoelectric coupling as the photonic pseudospin orbit interaction for left and right circularly polarized helical spin states. The Tellegen magnetoelectric coupling breaks bosonic time-reversal symmetry but instead gives rise to a conserved artificial fermionic-like-pseudo time-reversal symmetry, Tp ([Formula: see text]), due to the electromagnetic duality. Surprisingly, we find that, in this system, the helical edge states are, in fact, protected by this fermionic-like pseudo time-reversal symmetry Tp rather than by the bosonic time-reversal symmetry Tb This remarkable finding is expected to pave a new path to understanding the symmetry protection mechanism for topological phases of other fundamental particles and to searching for novel implementations for topological insulators.

The Parent Li(OH)FeSe Phase of Lithium Iron Hydroxide Selenide Superconductors.

Inorganic chemistry 55 (2016) 9886-9891

DN Woodruff, F Schild, CV Topping, SJ Cassidy, JN Blandy, SJ Blundell, AL Thompson, SJ Clarke

Lithiation of hydrothermally synthesized Li1-xFex(OH)Fe1-ySe turns on high-temperature superconductivity when iron ions are displaced from the hydroxide layers by reductive lithiation to fill the vacancies in the iron selenide layers. Further lithiation results in reductive iron extrusion from the hydroxide layers, which turns off superconductivity again as the stoichiometric composition Li(OH)FeSe is approached. The results demonstrate the twin requirements of stoichiometric FeSe layers and reduction of Fe below the +2 oxidation state as found in several iron selenide superconductors.

Studies of a Large Odd-Numbered Odd-Electron Metal Ring: Inelastic Neutron Scattering and Muon Spin Relaxation Spectroscopy of Cr8 Mn.

Chemistry (Weinheim an der Bergstrasse, Germany) 22 (2016) 1779-1788

ML Baker, T Lancaster, A Chiesa, G Amoretti, PJ Baker, C Barker, SJ Blundell, S Carretta, D Collison, HU Güdel, T Guidi, EJL McInnes, JS Möller, H Mutka, J Ollivier, FL Pratt, P Santini, F Tuna, PLW Tregenna-Piggott, IJ Vitorica-Yrezabal, GA Timco, REP Winpenny

The spin dynamics of Cr8 Mn, a nine-membered antiferromagnetic (AF) molecular nanomagnet, are investigated. Cr8 Mn is a rare example of a large odd-membered AF ring, and has an odd-number of 3d-electrons present. Odd-membered AF rings are unusual and of interest due to the presence of competing exchange interactions that result in frustrated-spin ground states. The chemical synthesis and structures of two Cr8 Mn variants that differ only in their crystal packing are reported. Evidence of spin frustration is investigated by inelastic neutron scattering (INS) and muon spin relaxation spectroscopy (μSR). From INS studies we accurately determine an appropriate microscopic spin Hamiltonian and we show that μSR is sensitive to the ground-spin-state crossing from S=1/2 to S=3/2 in Cr8 Mn. The estimated width of the muon asymmetry resonance is consistent with the presence of an avoided crossing. The investigation of the internal spin structure of the ground state, through the analysis of spin-pair correlations and scalar-spin chirality, shows a non-collinear spin structure that fluctuates between non-planar states of opposite chiralities.

On the temperature dependence of spin pumping in ferromagnet-topological insulator-ferromagnet spin valves

Results in Physics 6 (2016) 293-294

AA Baker, AI Figueroa, G van der Laan, T Hesjedal

Experimental and Theoretical Electron Density Analysis of Copper Pyrazine Nitrate Quasi-Low-Dimensional Quantum Magnets.

Journal of the American Chemical Society 138 (2016) 2280-2291

LHR Dos Santos, A Lanza, AM Barton, J Brambleby, WJA Blackmore, PA Goddard, F Xiao, RC Williams, T Lancaster, FL Pratt, SJ Blundell, J Singleton, JL Manson, P Macchi

The accurate electron density distribution and magnetic properties of two metal-organic polymeric magnets, the quasi-one-dimensional (1D) Cu(pyz)(NO3)2 and the quasi-two-dimensional (2D) [Cu(pyz)2(NO3)]NO3·H2O, have been investigated by high-resolution single-crystal X-ray diffraction and density functional theory calculations on the whole periodic systems and on selected fragments. Topological analyses, based on quantum theory of atoms in molecules, enabled the characterization of possible magnetic exchange pathways and the establishment of relationships between the electron (charge and spin) densities and the exchange-coupling constants. In both compounds, the experimentally observed antiferromagnetic coupling can be quantitatively explained by the Cu-Cu superexchange pathway mediated by the pyrazine bridging ligands, via a σ-type interaction. From topological analyses of experimental charge-density data, we show for the first time that the pyrazine tilt angle does not play a role in determining the strength of the magnetic interaction. Taken in combination with molecular orbital analysis and spin density calculations, we find a synergistic relationship between spin delocalization and spin polarization mechanisms and that both determine the bulk magnetic behavior of these Cu(II)-pyz coordination polymers.

Muon-spin relaxation study of the double perovskite insulators Sr2 BOsO6 (B  =  Fe, Y, ln).

Journal of physics. Condensed matter : an Institute of Physics journal 28 (2016) 076001-

RC Williams, F Xiao, IO Thomas, SJ Clark, T Lancaster, GA Cornish, SJ Blundell, W Hayes, AK Paul, C Felser, M Jansen

We present the results of zero-field muon-spin relaxation measurements made on the double perovskite insulators Sr2 BOsO6 (B = Fe,Y, In). Spontaneous muon-spin precession indicative of quasistatic long range magnetic ordering is observed in Sr2FeOsO6 within the AF1 antiferromagnetic phase for temperatures below [Formula: see text] K. Upon cooling below T2≈67 K the oscillations cease to be resolvable owing to the coexistence of the AF1 and AF2 phases, which leads to a broader range of internal magnetic fields. Using density functional calculations we identify a candidate muon stopping site within the unit cell, which dipole field simulations show to be consistent with the proposed magnetic structure. The possibility of incommensurate magnetic ordering is discussed for temperatures below TN = 53 K and 25 K for Sr2YOsO6 and Sr2InOsO6, respectively.

Detailed crystallographic analysis of the ice VI to ice XV hydrogen ordering phase transition.

The Journal of chemical physics 145 (2016) 204501-

CG Salzmann, B Slater, PG Radaelli, JL Finney, JJ Shephard, M Rosillo-Lopez, J Hindley

The D2O ice VI to ice XV hydrogen ordering phase transition at ambient pressure is investigated in detail with neutron diffraction. The lattice constants are found to be sensitive indicators for hydrogen ordering. The a and b lattice constants contract whereas a pronounced expansion in c is found upon hydrogen ordering. Overall, the hydrogen ordering transition goes along with a small increase in volume, which explains why the phase transition is more difficult to observe upon cooling under pressure. Slow-cooling ice VI at 1.4 GPa gives essentially fully hydrogen-disordered ice VI. Consistent with earlier studies, the ice XV obtained after slow-cooling at ambient pressure is best described with P-1 space group symmetry. Using a new modelling approach, we achieve the atomistic reconstruction of a supercell structure that is consistent with the average partially ordered structure derived from Rietveld refinements. This shows that C-type networks are most prevalent in ice XV, but other structural motifs outside of the classifications of the fully hydrogen-ordered networks are identified as well. The recently proposed Pmmn structural model for ice XV is found to be incompatible with our diffraction data, and we argue that only structural models that are capable of describing full hydrogen order should be used.

Bimetallic MOFs (H3O)x[Cu(MF6)(pyrazine)2]·(4 - x)H2O (M = V4+, x = 0; M = Ga3+, x = 1): co-existence of ordered and disordered quantum spins in the V4+ system.

Chemical communications (Cambridge, England) 52 (2016) 12653-12656

JL Manson, JA Schlueter, KE Garrett, PA Goddard, T Lancaster, JS Möller, SJ Blundell, AJ Steele, I Franke, FL Pratt, J Singleton, J Bendix, SH Lapidus, M Uhlarz, O Ayala-Valenzuela, RD McDonald, M Gurak, C Baines

The title compounds are bimetallic MOFs containing [Cu(pyz)2]2+ square lattices linked by MF6n- octahedra. In each, only the Cu2+ spins exhibit long-range magnetic order below 3.5 K (M = V4+) and 2.6 K (M = Ga3+). The V4+ spins remain disordered down to 0.5 K.

Building Large-Domain Twisted Bilayer Graphene with van Hove Singularity.

ACS nano 10 (2016) 6725-6730

Z Tan, J Yin, C Chen, H Wang, L Lin, L Sun, J Wu, X Sun, H Yang, Y Chen, H Peng, Z Liu

Twisted bilayer graphene (tBLG) with van Hove Singularity (VHS) has exhibited novel twist-angle-dependent chemical and physical phenomena. However, scalable production of high-quality tBLG is still in its infancy, especially lacking the angle controlled preparation methods. Here, we report a facile approach to prepare tBLG with large domain sizes (>100 μm) and controlled twist angles by a clean layer-by-layer transfer of two constituent graphene monolayers. The whole process without interfacial polymer contamination in two monolayers guarantees the interlayer interaction of the π-bond electrons, which gives rise to the existence of minigaps in electronic structures and the consequent formation of VHSs in density of state. Such perturbation on band structure was directly observed by angle-resolved photoemission spectroscopy with submicrometer spatial resolution (micro-ARPES). The VHSs lead to a strong light-matter interaction and thus introduce ∼20-fold enhanced intensity of Raman G-band, which is a characteristic of high-quality tBLG. The as-prepared tBLG with strong light-matter interaction was further fabricated into high-performance photodetectors with selectively enhanced photocurrent generation (up to ∼6 times compared with monolayer in our device).