Publications


Magnetic order and enhanced exchange in the quasi-one-dimensional molecule-based antiferromagnet Cu(NO3)2(pyz)3.

Physical chemistry chemical physics : PCCP 21 (2019) 1014-1018

BM Huddart, J Brambleby, T Lancaster, PA Goddard, F Xiao, SJ Blundell, FL Pratt, J Singleton, P Macchi, R Scatena, AM Barton, JL Manson

The quasi-one-dimensional molecule-based Heisenberg antiferromagnet Cu(NO3)2(pyz)3 has an intrachain coupling J = 13.7(1) K () and exhibits a state of long-range magnetic order below TN = 0.105(1) K. The ratio of interchain to intrachain coupling is estimated to be |J'/J| = 3.3 × 10-3, demonstrating a high degree of isolation for the Cu chains.


Electromagnon excitation in cupric oxide measured by Fabry-Pérot enhanced terahertz Mueller matrix ellipsometry.

Scientific reports 9 (2019) 1353-

S Knight, D Prabhakaran, C Binek, M Schubert

Here we present the use of Fabry-Pérot enhanced terahertz (THz) Mueller matrix ellipsometry to measure an electromagnon excitation in monoclinic cupric oxide (CuO). As a magnetically induced ferroelectric multiferroic, CuO exhibits coupling between electric and magnetic order. This gives rise to special quasiparticle excitations at THz frequencies called electromagnons. In order to measure the electromagnons in CuO, we exploit single-crystal CuO as a THz Fabry-Pérot cavity to resonantly enhance the excitation's signature. This enhancement technique enables the complex index of refraction to be extracted. We observe a peak in the absorption coefficient near 0.705 THz and 215 K, which corresponds to the electromagnon excitation. This absorption peak is observed along only one major polarizability axis in the monoclinic a-c plane. We show the excitation can be represented using the Lorentz oscillator model, and discuss how these Lorentz parameters evolve with temperature. Our findings are in excellent agreement with previous characterizations by THz time-domain spectroscopy (THz-TDS), which demonstrates the validity of this enhancement technique.


Paramagnon dispersion in beta-FeSe observed by Fe L-edge resonant inelastic x-ray scattering

Physical review B: Condensed matter and materials physics American Physical Society (2019)

M Rahn, K Kummer, N Brookes, A Haghighirad, K Gilmore, ANDREW BOOTHROYD


Visualizing electronic quantum matter

in Springer Handbooks, (2019) 1369-1390

K Fujita, MH Hamidian, PO Sprau, SD Edkins, JCS Davis

© Springer Nature Switzerland AG 2019. Modern quantum materials support a wide variety of exotic and unanticipated states of quantum matter and differ radically in phenomenology from conventional systems such as metals, semiconductors, band insulators, and ferromagnets. For example, quantum materials exhibit states such as electron liquid crystals, fluids of fractionalized quantum particles, quantum-entangled spin liquids, and topologically protected composite quantum particles. However, predictive theory is not fully developed for these forms of electronic quantum matter (EQM) and exploratory empirical research is required to discover and understand their properties. One of the most powerful and productive new techniques to achieve this is direct visualization of EQM at the atomic scale. For EQM, as with many highly complex systems in nature, seeing is believing and understanding. Here we describe the experimental, theoretical and analysis techniques of atomic-resolution spectroscopic imaging scanning tunneling microscopy (SI-STM) that allow such complex and enigmatic electronic/magnetic states to be directly visualized, identified, and understood.


Structural and optical properties of Cs2AgBiBr6 double perovskite

ACS Energy Letters American Chemical Society 4 (2018) 299-305

L Schade, AD Wright, RD Johnson, M Dollmann, B Wenger, PK Nayak, D Prabhakaran, LM Herz, RJ Nicholas, HJ Snaith, PG Radaelli

We present a comprehensive study of the relationship between the crystal structure and optoelectronic properties of the double perovskite Cs2AgBiBr6, which has emerged as a promising candidate for photovoltaic devices. On the basis of single-crystal/powder X-ray diffraction and neutron powder diffraction, we have revealed the presence of a structural phase transition at Ts ≈ 122 K between the room-temperature cubic structure (space group Fm3̅m) and a new low-temperature tetragonal structure (I4/m). From reflectivity measurements we found that the peak exciton energy Eex ≈ 2.85 eV near the direct gap shifts proportionally to the tetragonal strain, which is consistent with the Eex being primarily controlled by a rotational degree of freedom of the crystal structure, thus by the angle Bi−Ag−Br. We observed the time-resolved photoluminescence kinetics and we found that, among the relaxation channels, a fast one is mainly present in the tetragonal phase, suggesting that its origin may lie in the formation of tetragonal twin domains.


Role of defects in determining the magnetic ground state of ytterbium titanate.

Nature communications 10 (2019) 637-

DF Bowman, E Cemal, T Lehner, AR Wildes, L Mangin-Thro, GJ Nilsen, MJ Gutmann, DJ Voneshen, D Prabhakaran, AT Boothroyd, DG Porter, C Castelnovo, K Refson, JP Goff

Pyrochlore systems are ideally suited to the exploration of geometrical frustration in three dimensions, and their rich phenomenology encompasses topological order and fractional excitations. Classical spin ices provide the first context in which it is possible to control emergent magnetic monopoles, and anisotropic exchange leads to even richer behaviour associated with large quantum fluctuations. Whether the magnetic ground state of Yb2Ti2O7 is a quantum spin liquid or a ferromagnetic phase induced by a Higgs transition appears to be sample dependent. Here we have determined the role of structural defects on the magnetic ground state via the diffuse scattering of neutrons. We find that oxygen vacancies stabilise the spin liquid phase and the stuffing of Ti sites by Yb suppresses it. Samples in which the oxygen vacancies have been eliminated by annealing in oxygen exhibit a transition to a ferromagnetic phase, and this is the true magnetic ground state.


Rare earth doping of topological insulators: A brief review of thin film and heterostructure systems

physica status solidi (a) Wiley 216 (2019) 1800726-

T Hesjedal

Magnetic topological insulators (MTIs) are a novel materials class in which a topologically nontrivial electronic band structure coexists with long‐range ferromagnetic order. The ferromagnetic ground state can break time‐reversal symmetry, opening a gap in the topological surface states whose size is dependent on the magnitude of the magnetic moment. Doping with rare earth ions is one way to introduce higher magnetic moments into a material, however, in Bi2Te3 bulk crystals, the solubility limit is only a few percent. Using molecular beam epitaxy for the growth of doped (Sb,Bi)2(Se,Te)3 TI thin films, high doping concentrations can be achieved while preserving their high crystalline quality. The growth, structural, electronic, and magnetic properties of Dy, Ho, and Gd doped TI thin films will be reviewed. Indeed, high magnetic moments can be introduced into the TIs, which are, however, not ferromagnetically ordered. By making use of interfacial effects, magnetic long‐range order in Dy doped Bi2Te3, proximity‐coupled to the MTI Cr:Sb2Te3, has been achieved. Clearly, engineered MTI heterostructures offer new possibilities that combine the advantageous properties of different layers, and thus provide an ideal materials platform enabling the observation new quantum effects at higher temperatures.


Transverse and longitudinal spin-fluctuations in INVAR Fe0.65Ni0.35

Journal of Physics: Condensed Matter IOP Publishing 31 (2018) 025802

Stewart, Giblin, D Honecker, P Fouquet, D Prabhakaran, JW Taylor

The presence of spin-fluctuations deep within the ordered state of ferromagnetic [Formula: see text] alloy [Formula: see text] has long been suspected but seldom directly observed. Inhomogeneities of one type or another have been cited as important in stabilizing [Formula: see text] behaviour-either longitudinal spin-fluctuations associated with the [Formula: see text]-state (local environment) model or transverse magnetisation arising from non-collinear spin structures. In this study we employ small-angle neutron scattering with neutron polarization analysis to distinguish between the two possibilities. Surprisingly we in fact find evidence of dominant but uncorrelated longitudinal spin-fluctuations coexisting with transverse magnetisation which exists in short-range clusters of size ~[Formula: see text]. This finding supports recent first principles calculations of [Formula: see text] in which both longitudinal spin-fluctuations and magnetic short-range order are identified as important ingredients in reproducing the equilibrium [Formula: see text] lattice.


Influence of the support on stabilizing local defects in strained monolayer oxide films

Nanoscale Royal Society of Chemistry 11 (2019) 2412-2422

S Wang, X Hu, J Goniakowski, C Noguera, M Castell

Two-dimensional materials with a honeycomb lattice, such as graphene and hexagonal boron nitride, often contain local defects in which the hexagonal elements are replaced by four-, five-, seven-, and eight-membered rings. An example is the Stone-Wales (S-W) defect, where a bond rotation causes four hexagons to be transformed into a cluster of two pentagons and two heptagons. A further series of similar defects incorporating divacancies results in larger structures of non-hexagonal elements. In this paper, we use scanning tunneling microscopy (STM) and density functional theory (DFT) modeling to investigate the structure and energetics of S-W and divacancy defects in a honeycomb (2 × 2) Ti2O3 monolayer grown on an Au(111) substrate. The epitaxial rumpled Ti2O3 monolayer is pseudomorphic and in a state of elastic compression. As a consequence, divacancy defects, which induce tension in freestanding films, relieve the compression in the epitaxial Ti2O3 monolayer and therefore have significantly lower energies when compared with their freestanding counterparts. We find that at the divacancy defect sites there is a local reduction of the charge transfer between the film and the substrate, the rumpling is reduced, and the film has an increased separation from the substrate. Our results demonstrate the capacity of the substrate to significantly influence the energetics, and hence favor vacancy-type defects, in compressively strained 2D materials. This approach could be applied more broadly, for example to tensile monolayers, where vacancy-type defects would be rare and interstitial-type defects might be favored.


Skyrmions in anisotropic magnetic fields: strain and defect driven dynamics

MRS Advances Cambridge University Press 4 (2019) 643-650

R Brearton, S Zhang, MW Olszewski, G Van Der Laan, CJO Reichardt, C Reichardt, Eskildsen, T Hesjedal

Magnetic skyrmions are particle-like, topologically protected magnetization entities that are promising candidates for information carriers in racetrack-memory schemes. The transport of skyrmions in a shift-register-like fashion is crucial for their embodiment in practical devices. Recently, we demonstrated experimentally that chiral skyrmions in Cu2OSeO3 can be effectively manipulated by a magnetic field gradient, leading to a collective rotation of the skyrmion lattice with well-defined dynamics in a radial field gradient. Here, we employ a skyrmion particle model to numerically study the effects of resultant shear forces on the structure of the skyrmion lattice. We demonstrate that anisotropic peak broadening in experimentally observed diffraction patterns can be attributed to extended linear regions in the magnetic field profile. We show that topological (5-7) defects emerge to protect the six-fold symmetry of the lattice under the application of local shear forces, further enhancing the stability of proposed magnetic field driven devices.


A.C. susceptibility as a probe of low-frequency magnetic dynamics

Journal of Physics: Condensed Matter IOP Publishing 31 (2018)

C Topping, S Blundell

The experimental technique of a.c. susceptibility can be used as a probe of magnetic dynamics in a wide variety of systems. Its use is restricted to the low- frequency regime and thus is sensitive to relatively slow processes. Rather than measuring the dynamics of single spins, a.c. susceptibility can be used to probe the dynamics of collective objects, such as domain walls in ferromagnets or vortex matter in superconductors. In some frustrated systems, such as spin glasses, the complex interactions lead to substantial spectral weight of fluctuations in the low-frequency regime, and thus a.c. susceptibility can play a unique role. We review the theory underlying the technique and magnetic dynamics more generally and give applications of a.c. susceptibility to a wide variety of experimental situations.


Evolution of the low-temperature Fermi surface of superconducting FeSe1−xSx across a nematic phase transition

Nature npj Quantum Materials Springer Nature 4 (2019) 2

AI Coldea, SF Blake, S Kasahara, AA Haghighirad, MD Watson, W Knafo, ES Choi, A McCollam, P Reiss, T Yamashita, M Bruma, SC Speller, Y Matsuda, T Wolf, T Shibauchi, AJ Schofield


Phase transitions, broken symmetry and the renormalization group

in The Routledge Handbook of Emergence, (2019) 237-247

SJ Blundell

© 2019 selection and editorial matter, Sophie Gibb, Robin Findlay Hendry, and Tom Lancaster. All rights reserved. The renormalization group should probably be called the renormalization semigroup, but sometimes, contradictory terminology sticks. The renormalization group procedure provides important insights because it shows quantitatively how fine-scale structure is progressively ignored and the physics of critical phenomena depend on these larger-scale, what students might call "structural", features of the theory. The renormalization group breaks big problems down into small ones. Broken symmetry can be seen as a well-studied paradigm of emergent behaviour in the physical world. By breaking symmetry, these phases forfeit the status of being a "stationary state" of the sort beloved of elementary quantum mechanics treatments. Phase transitions are sharp and there is a clear delineation between the ordered and disordered states. The set of symmetry-breaking phase transitions includes as members those between the ferromagnetic and paramagnetic states and those between the superconducting and normal metal states of certain materials.


Monitoring ultrafast metallization in LaCoO3 with femtosecond soft x-ray spectroscopy

COMMUNICATIONS PHYSICS 2 (2019) ARTN 8

M Izquierdo, M Karolak, D Prabhakaran, AT Boothroyd, AO Scherz, A Lichtenstein, SL Molodtsov


Systematic study of ferromagnetism in CrxSb2-xTe3 topological insulator thin films using electrical and optical techniques

Scientific Reports Springer Nature 8 (2018) 17024

A Singh, V Kamboj, J Liu, J Llandro, L Duffy, SP Senanayak, HE Beere, A Ionescu, DA Ritchie, T Hesjedal, CHW Barnes

Ferromagnetic ordering in a topological insulator can break time-reversal symmetry, realizing dissipationless electronic states in the absence of a magnetic field. The control of the magnetic state is of great importance for future device applications. We provide a detailed systematic study of the magnetic state in highly doped CrxSb2−xTe3 thin films using electrical transport, magneto-optic Kerr effect measurements and terahertz time domain spectroscopy, and also report an efficient electric gating of ferromagnetic order using the electrolyte ionic liquid [DEME][TFSI]. Upon increasing the Cr concentration from x = 0.15 to 0.76, the Curie temperature (Tc) was observed to increase by ~5 times to 176 K. In addition, it was possible to modify the magnetic moment by up to 50% with a gate bias variation of just ±3 V, which corresponds to an increase in carrier density by 50%. Further analysis on a sample with x = 0.76 exhibits a clear insulator-metal transition at Tc, indicating the consistency between the electrical and optical measurements. The direct correlation obtained between the carrier density and ferromagnetism - in both electrostatic and chemical doping - using optical and electrical means strongly suggests a carrier-mediated Ruderman-Kittel-Kasuya-Yoshida (RKKY) coupling scenario. Our low-voltage means of manipulating ferromagnetism, and consistency in optical and electrical measurements provides a way to realize exotic quantum states for spintronic and low energy magneto-electronic device applications.


Helical magnetism in Sr-doped CaMn7O12 films

PHYSICAL REVIEW B 98 (2018) ARTN 224419

A Huon, AM Vibhakar, AJ Grutter, JA Borchers, S Disseler, Y Liu, W Tian, F Orlandi, P Manuel, DD Khalyavin, Y Sharma, A Herklotz, HN Lee, MR Fitzsimmons, RD Johnson, SJ May


Common glass-forming spin-liquid state in the pyrochlore magnets Dy2Ti2 O7 and Ho2Ti2 O7

Physical Review B 98 (2018)

AB Eyvazov, R Dusad, TJS Munsie, HA Dabkowska, GM Luke, ER Kassner, JCS Davis, A Eyal

© 2018 American Physical Society. Despite a well-ordered pyrochlore crystal structure and strong magnetic interactions between the Dy3+ or Ho3+ ions, no long-range magnetic order has been detected in the pyrochlore titanates Ho2Ti2O7 and Dy2Ti2O7. To explore the actual magnetic phase formed by cooling these materials, we measure their magnetization dynamics using toroidal, boundary-free magnetization transport techniques. We find that the dynamical magnetic susceptibility of both compounds has the same distinctive phenomenology, which is indistinguishable in form from that of the dielectric permittivity of dipolar glass-forming liquids. Moreover, Ho2Ti2O7 and Dy2Ti2O7 both exhibit microscopic magnetic relaxation times that increase along the super-Arrhenius trajectories analogous to those observed in glass-forming dipolar liquids. Thus, upon cooling below about 2 K, Dy2Ti2O7 and Ho2Ti2O7 both appear to enter the same magnetic state exhibiting the characteristics of a glass-forming spin liquid.


Phase diagram of Bi2Sr2CaCu2O8+δ revisited.

Nature communications 9 (2018) 5210-

IK Drozdov, I Pletikosić, C-K Kim, K Fujita, GD Gu, JCS Davis, PD Johnson, I Božović, T Valla

In cuprate superconductors, the doping of carriers into the parent Mott insulator induces superconductivity and various other phases whose characteristic temperatures are typically plotted versus the doping level p. In most materials, p cannot be determined from the chemical composition, but it is derived from the superconducting transition temperature, Tc, using the assumption that the Tc dependence on doping is universal. Here, we present angle-resolved photoemission studies of Bi2Sr2CaCu2O8+δ, cleaved and annealed in vacuum or in ozone to reduce or increase the doping from the initial value corresponding to Tc = 91 K. We show that p can be determined from the underlying Fermi surfaces and that in-situ annealing allows mapping of a wide doping regime, covering the superconducting dome and the non-superconducting phase on the overdoped side. Our results show a surprisingly smooth dependence of the inferred Fermi surface with doping. In the highly overdoped regime, the superconducting gap approaches the value of 2Δ0 = (4 ± 1)kBTc.


Significant change in the electronic behavior associated with structural distortions in monocrystalline SrAg4As2

PHYSICAL REVIEW B 98 (2018) ARTN 235130

B Shen, E Emmanouilidou, X Deng, A McCollam, J Xing, G Kotliar, AI Coldea, N Ni


Multigap Superconductivity in RbCa2Fe4As4F2 Investigated Using mu SR Measurements

JOURNAL OF THE PHYSICAL SOCIETY OF JAPAN 87 (2018) ARTN 124705

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

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