Publications


Static and fluctuating magnetic moments in the ferroelectric metal LiOsO3

JPS Conference Proceedings Physical Society of Japan 日本物理学会 21 (2018) 1-6

F Kirschner, F Lang, FL Pratt, T Lancaster, Y Shi, Y Guo, A Boothroyd, S Blundell

LiOsO3 is the first example of a new class of material called a ferroelectric metal. We performed zero-field and longitudinal-field μSR, along with a combination of electronic structure and dipole field calculations, to determine the magneticground state of LiOsO3. We find that the sample contains both static Li nuclear moments and dynamic Os electronic moments. Below ≈0.7 K, the fluctuations of the Os moments slow down, though remain dynamic down to 0.08 K. We expect this could result in a frozen-out, disordered ground state at even lower temperatures.


Nodal multigap superconductivity in KCa2Fe4As4F2

Physical Review B 97 (2018) 060509(R)

M Smidman, FKK Kirschner, DT Adroja, AD Hillier, F Lang, Z-C Zhang, G-H Cao, SJ Blundell


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.


Extreme sensitivity of a topochemical reaction to cation substitution: SrVO2H versus SrV1-xTixO1.5H1.5

Inorganic Chemistry American Chemical Society 57 (2018) 2890–2898-

M Amano Patino, D Zeng, J McGrady, S Blundell, M Hayward

The anion-ordered oxide-hydride SrVO2H is an antiferromagnetic insulator due to strong correlations between vanadium d electrons. In an attempt to hole-dope SrVO2H into a metallic state, a strategy of first preparing SrV1-xTixO3 phases and then converting them to the corresponding SrV1-xTixO2H phases via reaction with CaH2 was followed. This revealed that the solid solution between SrVO3 and SrTiO3 is only stable at high temperature. In addition, reactions between SrV0.95Ti0.05O3 and CaH2 were observed to yield SrV0.95Ti0.05O1.5H1.5 not SrV0.95Ti0.05O2H. This dramatic change in reactivity for a very modest change in initial chemical composition is attributed to an electronic destabilization of SrVO2H on titanium substitution. Density functional theory calculations indicate that the presence of an anion-ordered, tetragonal SrMO2H phase is uniquely associated with a d2 electron count and that titanium substitution leads to an electronic destabilization of SrV1-xTixO2H phases, which, ultimately, drives further reaction of SrV1-xTixO2H to SrV1-xTixO1.5H1.5. The observed sensitivity of the reaction products to the chemical composition of initial phases highlights some of the difficulties associated with electronically doping metastable materials prepared by topochemical reactions.


LaSr3 NiRuO4 H4 : A 4d Transition-Metal Oxide-Hydride Containing Metal Hydride Sheets.

Angewandte Chemie (International ed. in English) (2018)

L Jin, M Lane, D Zeng, FKK Kirschner, F Lang, P Manuel, SJ Blundell, JE McGrady, MA Hayward

The synthesis of the first 4d transition metal oxide-hydride, LaSr3 NiRuO4 H4 , is prepared via topochemical anion exchange. Neutron diffraction data show that the hydride ions occupy the equatorial anion sites in the host lattice and as a result the Ru and Ni cations are located in a plane containing only hydride ligands, a unique structural feature with obvious parallels to the CuO2 sheets present in the superconducting cuprates. DFT calculations confirm the presence of S=1/2  Ni+ and S=0, Ru2+ centers, but neutron diffraction and μSR data show no evidence for long-range magnetic order between the Ni centers down to 1.8 K. The observed weak inter-cation magnetic coupling can be attributed to poor overlap between Ni 3dz2 and H 1s in the super-exchange pathways.


Comparative study of the magnetic properties of La3Ni2B'O9 for B' = Nb, Ta or Sb

Journal of Solid State Chemistry Elsevier 258 (2017) 825-834

C-M Chin, P Battle, SJ Blundell, EC Hunter, F Lang, R Paria Sena, M Hendrickx, J Hadermann

<p>Polycrystalline samples of La<sub>3</sub>Ni<sub>2</sub>NbO<sub>9</sub> and La<sub>3</sub>Ni<sub>2</sub>TaO<sub>9</sub> have been characterised by X-ray and neutron diffraction, electron microscopy, magnetometry and muon spin relaxation (µSR); the latter technique was also applied to La<sub>3</sub>Ni<sub>2</sub>SbO<sub>9</sub>. On the length scale of a neutron diffraction experiment, the six-coordinate sites of the monoclinic perovskite structure are occupied in a 1:1 ordered manner by Ni and a random ⅓Ni/⅔B’ mixture. Electron microscopy demonstrated that this 1:1 ordering is maintained over microscopic distances, although diffuse scattering indicative of short-range ordering on the mixed site was observed. No magnetic Bragg scattering was observed in neutron diffraction patterns collected from La<sub>3</sub>Ni<sub>2</sub>B’O<sub>9 </sub>(B’ = Nb or Ta) at 5 K although in each case µSR identified the presence of static spins below 30 K. Magnetometry showed that La<sub>3</sub>Ni<sub>2</sub>NbO<sub>9</sub> behaves as a spin glass below 29 K but significant short-range interactions are present in La<sub>3</sub>Ni<sub>2</sub>TaO<sub>9</sub> below 85 K. The contrasting properties of these compounds are discussed in terms of their microstructure.</p>


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

Nature communications (2018)

MOON-SUN Nam, B Williams, YULIN Chen, S Contera, S Yao, M Lu, YULIN Chen, GA Timco, CA Muryn, ARZHANG Ardavan

The original version of this Article contained an error in the spelling of the author Benjamin H. Williams, which was incorrectly given as Benjamin H. Willams. This has now been corrected in both the PDF and HTML versions of the Article.


How to probe the spin contribution to momentum relaxation in topological insulators (vol 8, 2017)

NATURE COMMUNICATIONS 9 (2018) ARTN 729

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


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

Nat Commun 9 (2018) 729-

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

The original version of this Article contained an error in the spelling of the author Benjamin H. Williams, which was incorrectly given as Benjamin H. Willams. This has now been corrected in both the PDF and HTML versions of the Article.


Two-gap superconductivity with line nodes in CsCa2Fe4As4F2

Physical Review B American Physical Society 97 (2018) 060506(R)-

F Kirschner, DT Adroja, F Lang, Z-W Wang, M Smidman, PJ Baker, G-H Cao, SJ Blundell

We report the results of a muon-spin rotation ($\mu$SR) experiment to determine the superconducting ground state of the iron-based superconductor $CsCa_2Fe_4As_4F_2$ with $T_{\rm c} \approx 28.3\,K$. This compound is related to the fully-gapped superconductor $CaCsFe_4As_4$, but here the Ca-containing spacer layer is replaced with one containing $Ca_2F_2$. The temperature evolution of the penetration depth strongly suggests the presence of line nodes and is best modelled by a system consisting of both an $s-$ and a $d-$wave gap. We also find a potentially magnetic phase which appears below $\approx 10\,K$ but does not appear to compete with the superconductivity. This compound contains the largest alkali atom in this family of superconductors and our results yield a value for the in-plane penetration depth of $\lambda_{ab}(T=0)=423(5)\,nm$.


In-situ angle-resolved photoemission spectroscopy of copper-oxide thin films synthesized by molecular beam epitaxy

Journal of Electron Spectroscopy and Related Phenomena (2018)

CK Kim, IK Drozdov, K Fujita, JCS Davis, I Božović, T Valla

© 2018 Elsevier B.V. Angle-resolved photoemission spectroscopy (ARPES) is the key momentum-resolved technique for direct probing of the electronic structure of a material. However, since it is highly surface-sensitive, it has been applied to a relatively small set of complex oxides that can be easily cleaved in ultra-high vacuum. Here we describe a new multi-module system at Brookhaven National Laboratory (BNL) in which an oxide molecular beam epitaxy (OMBE) is interconnected with an ARPES and a spectroscopic-imaging scanning tunneling microscopy (SI-STM) module. This new capability largely expands the range of complex-oxide materials and artificial heterostructures accessible to these two most powerful and complementary techniques for studies of electronic structure of materials. We also present the first experimental results obtained using this system — the ARPES studies of electronic band structure of a La2-xSrxCuO4 (LSCO) thin film grown by OMBE.


Emergence, causation and storytelling: condensed matter physics and the limitations of the human mind

Philosophica Department of Philosophy and Moral Science at Ghent University 92 (2018) 139-164

S Blundell

The physics of matter in the condensed state is concerned with problems in which the number of constituent particles is vastly greater than can be easily comprehended. The inherent physical limitations of the human mind are fundamental and restrict the way in which we can interact with and learn about the universe. This presents challenges for developing scientific explanations that are met by emergent narratives, concepts and arguments that have a non-trivial relationship to the underlying microphysics. By examining examples within condensed matter physics, and also from cellular automata, I show how such emergent narratives efficiently describe elements of reality.


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.


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

Nat Commun 9 (2018) 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.


Comparative study of the magnetic properties of La<inf>3</inf>Ni<inf>2</inf>B′O<inf>9</inf>for B′ = Nb, Taor Sb

Journal of Solid State Chemistry 258 (2018) 825-834

CM Chin, PD Battle, SJ Blundell, E Hunter, F Lang, M Hendrickx, R Paria Sena, J Hadermann

© 2017 Elsevier Inc. Polycrystalline samples of La 3 Ni 2 NbO 9 and La 3 Ni 2 TaO 9 have been characterised by X-ray and neutron diffraction, electron microscopy, magnetometry and muon spin relaxation (µSR); the latter technique was also applied to La 3 Ni 2 SbO 9 . On the length scale of a neutron diffraction experiment, the six-coordinate sites of the monoclinic perovskite structure are occupied in a 1:1 ordered manner by Ni and a random ⅓Ni/⅔B′ mixture. Electron microscopy demonstrated that this 1:1 ordering is maintained over microscopic distances, although diffuse scattering indicative of short-range ordering on the mixed site was observed. No magnetic Bragg scattering was observed in neutron diffraction patterns collected from La 3 Ni 2 B′O 9 (B′ = Nb or Ta) at 5 K although in each case µSR identified the presence of static spins below 30 K. Magnetometry showed that La 3 Ni 2 NbO 9 behaves as a spin glass below 29 K but significant short-range interactions are present in La 3 Ni 2 TaO 9 below 85 K. The contrasting properties of these compounds are discussed in terms of their microstructure.


Low-field spin dynamics of Cr7Ni and Cr7Ni-Cu-Cr7Ni molecular rings as detected by mu SR

PHYSICAL REVIEW B 96 (2017) ARTN 184403

S Sanna, P Arosio, L Bordonali, F Adelnia, M Mariani, E Garlatti, C Baines, A Amato, KPV Sabareesh, G Timco, REP Winpenny, SJ Blundell, A Lascialfari


Crystal structure and magnetic modulation in beta-Ce2O2FeSe2

PHYSICAL REVIEW MATERIALS 1 (2017) ARTN 034403

C-H Wang, CM Ainsworth, SD Champion, GA Stewart, MC Worsdale, T Lancaster, SJ Blundell, HEA Brand, JSO Evans


Local magnetism and spin dynamics of the frustrated honeycomb rhodate Li2RhO3

PHYSICAL REVIEW B 96 (2017) ARTN 094432

P Khuntia, S Manni, FR Foronda, T Lancaster, SJ Blundell, P Gegenwart, M Baenitz


Strong coupling of microwave photons to antiferromagnetic fluctuations in an organic magnet

Physical Review Letters American Physical Society 119 (2017) 147701-

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

Coupling between a crystal of di(phenyl)-(2,4,6-trinitrophenyl)iminoazanium (DPPH) radicals and a superconducting microwave resonator is investigated in a circuit quantum electrodynamics (cQED) 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 multi-spin modes in organic crystals are suitable for cQED, offering a platform for their coherent manipulation. They also utilize the cQED architecture as a way to probe spin correlations at low temperature.


The spin resonance clock transition of the endohedral fullerene $^{15}\mathrm{N@C}_{60}$

Physical Review Letters American Physical Society 119 (2017) 140801-

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

The endohedral fullerene $^{15}\mathrm{N@C}_{60}$ 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.

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