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

Nat Commun 9 (0) 56-

M-S Nam, BH Willams, 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.

Coexistence of magnetism and superconductivity in separate layers of the iron-based superconductor Li1-xFex(OH)Fe1-ySe

PHYSICAL REVIEW B 95 (2017) ARTN 134419

CV Topping, FKK Kirschner, SJ Blundell, PJ Baker, DN Woodruff, F Schild, H Sun, SJ Clarke

Room-temperature helimagnetism in FeGe thin films.

Scientific reports 7 (2017) 123-

SL Zhang, I Stasinopoulos, T Lancaster, F Xiao, A Bauer, F Rucker, AA Baker, AI Figueroa, Z Salman, FL Pratt, SJ Blundell, T Prokscha, A Suter, J Waizner, M Garst, D Grundler, G van der Laan, C Pfleiderer, T Hesjedal

Chiral magnets are promising materials for the realisation of high-density and low-power spintronic memory devices. For these future applications, a key requirement is the synthesis of appropriate materials in the form of thin films ordering well above room temperature. Driven by the Dzyaloshinskii-Moriya interaction, the cubic compound FeGe exhibits helimagnetism with a relatively high transition temperature of 278 K in bulk crystals. We demonstrate that this temperature can be enhanced significantly in thin films. Using x-ray scattering and ferromagnetic resonance techniques, we provide unambiguous experimental evidence for long-wavelength helimagnetic order at room temperature and magnetic properties similar to the bulk material. We obtain α intr = 0.0036 ± 0.0003 at 310 K for the intrinsic damping parameter. We probe the dynamics of the system by means of muon-spin rotation, indicating that the ground state is reached via a freezing out of slow dynamics. Our work paves the way towards the fabrication of thin films of chiral magnets that host certain spin whirls, so-called skyrmions, at room temperature and potentially offer integrability into modern electronics.

Strong Coupling of Microwave Photons to Antiferromagnetic Fluctuations in an Organic Magnet.

Physical review letters 119 (2017) 147701-

M Mergenthaler, J Liu, JJ Le Roy, N Ares, AL Thompson, L Bogani, F Luis, SJ Blundell, T Lancaster, A Ardavan, GAD Briggs, PJ Leek, EA Laird

Coupling between a crystal of di(phenyl)-(2,4,6-trinitrophenyl)iminoazanium radicals and a superconducting microwave resonator is investigated in a circuit quantum electrodynamics (circuit QED) architecture. The crystal exhibits paramagnetic behavior above 4 K, with antiferromagnetic correlations appearing below this temperature, and we demonstrate strong coupling at base temperature. The magnetic resonance acquires a field angle dependence as the crystal is cooled down, indicating anisotropy of the exchange interactions. These results show that multispin modes in organic crystals are suitable for circuit QED, offering a platform for their coherent manipulation. They also utilize the circuit QED architecture as a way to probe spin correlations at low temperature.

Quantum-critical spin dynamics in a Tomonaga-Luttinger liquid studied with muon-spin relaxation

PHYSICAL REVIEW B 95 (2017) ARTN 020402

JS Moller, T Lancaster, SJ Blundell, FL Pratt, PJ Baker, F Xiao, RC Williams, W Hayes, MM Turnbul, CP Landee

Spin Resonance Clock Transition of the Endohedral Fullerene ^{15}N@C_{60}.

Physical review letters 119 (2017) 140801-

RT Harding, S Zhou, J Zhou, T Lindvall, WK Myers, A Ardavan, GAD Briggs, K Porfyrakis, EA Laird

The endohedral fullerene ^{15}N@C_{60} has narrow electron paramagnetic resonance lines which have been proposed as the basis for a condensed-matter portable atomic clock. We measure the low-frequency spectrum of this molecule, identifying and characterizing a clock transition at which the frequency becomes insensitive to magnetic field. We infer a linewidth at the clock field of 100 kHz. Using experimental data, we are able to place a bound on the clock's projected frequency stability. We discuss ways to improve the frequency stability to be competitive with existing miniature clocks.

La2SrCr2O7: Controlling the Tilting Distortions of n = 2 Ruddlesden-Popper Phases through A-Site Cation Order.

Inorganic chemistry 55 (2016) 8951-8960

R Zhang, BM Abbett, G Read, F Lang, T Lancaster, TT Tran, PS Halasyamani, SJ Blundell, NA Benedek, MA Hayward

Structural characterization by neutron diffraction, supported by magnetic, SHG, and μ(+)SR data, reveals that the n = 2 Ruddlesden-Popper phase La2SrCr2O7 adopts a highly unusual structural configuration in which the cooperative rotations of the CrO6 octahedra are out of phase in all three Cartesian directions (ΦΦΦz/ΦΦΦz; a(-)a(-)c(-)/a(-)a(-)c(-)) as described in space group A2/a. First-principles DFT calculations indicate that this unusual structural arrangement can be attributed to coupling between the La/Sr A-site distribution and the rotations of the CrO6 units, which combine to relieve the local deformations of the chromium-oxygen octahedra. This coupling suggests new chemical "handles" by which the rotational distortions or A-site cation order of Ruddlesden-Popper phases can be directed to optimize physical behavior. Low-temperature neutron diffraction data and μ(+)SR data indicate La2SrCr2O7 adopts a G-type antiferromagnetically ordered state below TN ∼ 260 K.

Making hybrid [n]-rotaxanes as supramolecular arrays of molecular electron spin qubits.

Nature communications 7 (2016) 10240-

A Fernandez, J Ferrando-Soria, EM Pineda, F Tuna, IJ Vitorica-Yrezabal, C Knappke, J Ujma, CA Muryn, GA Timco, PE Barran, A Ardavan, REP Winpenny

Quantum information processing (QIP) would require that the individual units involved--qubits--communicate to other qubits while retaining their identity. In many ways this resembles the way supramolecular chemistry brings together individual molecules into interlocked structures, where the assembly has one identity but where the individual components are still recognizable. Here a fully modular supramolecular strategy has been to link hybrid organic-inorganic [2]- and [3]-rotaxanes into still larger [4]-, [5]- and [7]-rotaxanes. The ring components are heterometallic octanuclear [Cr7NiF8(O2C(t)Bu)16](-) coordination cages and the thread components template the formation of the ring about the organic axle, and are further functionalized to act as a ligand, which leads to large supramolecular arrays of these heterometallic rings. As the rings have been proposed as qubits for QIP, the strategy provides a possible route towards scalable molecular electron spin devices for QIP. Double electron-electron resonance experiments demonstrate inter-qubit interactions suitable for mediating two-qubit quantum logic gates.

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

Fourier space derivation of the demagnetization tensor for uniformly magnetized objects of cylindrical symmetry


F Lang, SJ Blundell

Quantum Interference in Graphene Nanoconstrictions.

Nano letters 16 (2016) 4210-4216

P Gehring, H Sadeghi, S Sangtarash, CS Lau, J Liu, A Ardavan, JH Warner, CJ Lambert, GAD Briggs, JA Mol

We report quantum interference effects in the electrical conductance of chemical vapor deposited graphene nanoconstrictions fabricated using feedback controlled electroburning. The observed multimode Fabry-Pérot interferences can be attributed to reflections at potential steps inside the channel. Sharp antiresonance features with a Fano line shape are observed. Theoretical modeling reveals that these Fano resonances are due to localized states inside the constriction, which couple to the delocalized states that also give rise to the Fabry-Pérot interference patterns. This study provides new insight into the interplay between two fundamental forms of quantum interference in graphene nanoconstrictions.

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.

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.

Bimetallic MOFs (H3O)x[Cu(MF6)(pyrazine)2]·(4 - x)H2O (M = V(4+), x = 0; M = Ga(3+), x = 1): co-existence of ordered and disordered quantum spins in the V(4+) 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 MF6(n-) octahedra. In each, only the Cu(2+) spins exhibit long-range magnetic order below 3.5 K (M = V(4+)) and 2.6 K (M = Ga(3+)). The V(4+) spins remain disordered down to 0.5 K.

La2SrCr2O7F2: A Ruddlesden-Popper Oxyfluoride Containing Octahedrally Coordinated Cr(4+) Centers.

Inorganic chemistry 55 (2016) 3169-3174

R Zhang, G Read, F Lang, T Lancaster, SJ Blundell, MA Hayward

The low-temperature fluorination of the n = 2 Ruddlesden-Popper phase La2SrCr2O7 yields La2SrCr2O7F2 via a topochemical fluorine insertion reaction. The structure-conserving nature of the fluorination reaction means that the chromium centers of the initial oxide phase retain an octahedral coordination environment in the fluorinated product, resulting in a material containing an extended array of apex-linked Cr(4+)O6 units. Typically materials containing networks of octahedrally coordinated Cr(4+) centers can only be prepared at high pressure; thus, the preparation of La2SrCr2O7F2 demonstrates that low-temperature topochemical reactions offer an alternative synthesis route to materials of this type. Neutron diffraction, magnetization, and μ(+)SR data indicate that La2SrCr2O7F2 undergoes a transition to an antiferromagnetic state below TN ≈ 140 K. The structure-property relations of this phase and other Cr(4+) oxide phases are discussed.

Ordering Gold Nanoparticles with DNA Origami Nanoflowers.

ACS nano 10 (2016) 7303-7306

R Schreiber, I Santiago, A Ardavan, AJ Turberfield

Nanostructured materials, including plasmonic metamaterials made from gold and silver nanoparticles, provide access to new materials properties. The assembly of nanoparticles into extended arrays can be controlled through surface functionalization and the use of increasingly sophisticated linkers. We present a versatile way to control the bonding symmetry of gold nanoparticles by wrapping them in flower-shaped DNA origami structures. These "nanoflowers" assemble into two-dimensonal gold nanoparticle lattices with symmetries that can be controlled through auxiliary DNA linker strands. Nanoflower lattices are true composites: interactions between the gold nanoparticles are mediated entirely by DNA, and the DNA origami will fold into its designed form only in the presence of the gold nanoparticles.

Transverse field muon-spin rotation measurement of the topological anomaly in a thin film of MnSi

PHYSICAL REVIEW B 93 (2016) ARTN 140412

T Lancaster, F Xiao, Z Salman, IO Thomas, SJ Blundell, FL Pratt, SJ Clark, T Prokscha, A Suter, SL Zhang, AA Baker, T Hesjedal

Nanoscale depth-resolved polymer dynamics probed by the implantation of low energy muons

POLYMER 105 (2016) 516-525

FL Pratt, T Lancaster, PJ Baker, SJ Blundell, T Prokscha, E Morenzoni, A Suter, HE Assender