Publications


Evidence for a J(eff)=0 ground state and defect-induced spin glass behavior in the pyrochlore osmate Y2Os2O7

PHYSICAL REVIEW B 99 (2019) ARTN 174442

NR Davies, CV Topping, H Jacobsen, AJ Princep, FKK Kirschner, MC Rahn, M Bristow, JG Vale, I da Silva, PJ Baker, CJ Sahle, Y-F Guo, D-Y Yan, Y-G Shi, SJ Blundell, DF McMorrow, AT Boothroyd


Magnetic field-induced pair density wave state in the cuprate vortex halo.

Science (New York, N.Y.) 364 (2019) 976-980

SD Edkins, A Kostin, K Fujita, AP Mackenzie, H Eisaki, S Uchida, S Sachdev, MJ Lawler, E-A Kim, JC Séamus Davis, MH Hamidian

High magnetic fields suppress cuprate superconductivity to reveal an unusual density wave (DW) state coexisting with unexplained quantum oscillations. Although routinely labeled a charge density wave (CDW), this DW state could actually be an electron-pair density wave (PDW). To search for evidence of a field-induced PDW, we visualized modulations in the density of electronic states N(r) within the halo surrounding Bi2Sr2CaCu2O8 vortex cores. We detected numerous phenomena predicted for a field-induced PDW, including two sets of particle-hole symmetric N(r) modulations with wave vectors QP and 2QP , with the latter decaying twice as rapidly from the core as the former. These data imply that the primary field-induced state in underdoped superconducting cuprates is a PDW, with approximately eight CuO2 unit-cell periodicity and coexisting with its secondary CDWs.


Probing magnetic order and disorder in the one-dimensional molecular spin chains CuF2(pyz) and [Ln(hfac)3(boaDTDA)] n (Ln  =  Sm, La) using implanted muons.

Journal of physics. Condensed matter : an Institute of Physics journal 31 (2019) 394002-394002

T Lancaster, BM Huddart, RC Williams, F Xiao, KJA Franke, PJ Baker, FL Pratt, SJ Blundell, JA Schlueter, MB Mills, AC Maahs, KE Preuss

We present the results of muon-spin relaxation ([Formula: see text]SR) measurements on antiferromagnetic and ferromagnetic spin chains. In antiferromagnetic CuF2(pyz) we identify a transition to long range magnetic order taking place at [Formula: see text] K, allowing us to estimate a ratio with the intrachain exchange of [Formula: see text] and the ratio of interchain to intrachain exchange coupling as [Formula: see text]. The ferromagnetic chain [Sm(hfac)3(boaDTDA)] n undergoes an ordering transition at [Formula: see text] K, seen via a broad freezing of dynamic fluctuations on the muon (microsecond) timescale and implying [Formula: see text]. The ordered radical moment continues to fluctuate on this timescale down to 0.3 K, while the Sm moments remain disordered. In contrast, the radical spins in [La(hfac)3(boaDTDA)] n remain magnetically disordered down to T  =  0.1 K suggesting [Formula: see text].


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.


Local magnetism, magnetic order and spin freezing in the 'nonmetallic metal' FeCrAs.

Journal of physics. Condensed matter : an Institute of Physics journal 31 (2019) 285803-285803

BM Huddart, MT Birch, FL Pratt, SJ Blundell, DG Porter, SJ Clark, W Wu, SR Julian, PD Hatton, T Lancaster

We present the results of x-ray scattering and muon-spin relaxation ([Formula: see text]SR) measurements on the iron-pnictide compound FeCrAs. Polarized non-resonant magnetic x-ray scattering results reveal the 120° periodicity expected from the suggested three-fold symmetric, non-collinear antiferromagnetic structure. [Formula: see text]SR measurements indicate a magnetically ordered phase throughout the bulk of the material below [Formula: see text] K. There are signs of fluctuating magnetism in a narrow range of temperatures above [Formula: see text] involving low-energy excitations, while at temperatures well below [Formula: see text] behaviour characteristic of freezing of dynamics is observed, likely reflecting the effect of disorder in our polycrystalline sample. Using density functional theory we propose a distinct muon stopping site in this compound and assess the degree of distortion induced by the implanted muon.


Machine learning in electronic-quantum-matter imaging experiments.

Nature 570 (2019) 484-490

Y Zhang, A Mesaros, K Fujita, SD Edkins, MH Hamidian, K Ch'ng, H Eisaki, S Uchida, JCS Davis, E Khatami, E-A Kim

For centuries, the scientific discovery process has been based on systematic human observation and analysis of natural phenomena1. Today, however, automated instrumentation and large-scale data acquisition are generating datasets of such large volume and complexity as to defy conventional scientific methodology. Radically different scientific approaches are needed, and machine learning (ML) shows great promise for research fields such as materials science2-5. Given the success of ML in the analysis of synthetic data representing electronic quantum matter (EQM)6-16, the next challenge is to apply this approach to experimental data-for example, to the arrays of complex electronic-structure images17 obtained from atomic-scale visualization of EQM. Here we report the development and training of a suite of artificial neural networks (ANNs) designed to recognize different types of order hidden in such EQM image arrays. These ANNs are used to analyse an archive of experimentally derived EQM image arrays from carrier-doped copper oxide Mott insulators. In these noisy and complex data, the ANNs discover the existence of a lattice-commensurate, four-unit-cell periodic, translational-symmetry-breaking EQM state. Further, the ANNs determine that this state is unidirectional, revealing a coincident nematic EQM state. Strong-coupling theories of electronic liquid crystals18,19 are consistent with these observations.


Evidence for a vestigial nematic state in the cuprate pseudogap phase.

Proceedings of the National Academy of Sciences of the United States of America 116 (2019) 13249-13254

S Mukhopadhyay, R Sharma, CK Kim, SD Edkins, MH Hamidian, H Eisaki, S-I Uchida, E-A Kim, MJ Lawler, AP Mackenzie, JCS Davis, K Fujita

The CuO2 antiferromagnetic insulator is transformed by hole-doping into an exotic quantum fluid usually referred to as the pseudogap (PG) phase. Its defining characteristic is a strong suppression of the electronic density-of-states D(E) for energies |E| < [Formula: see text], where [Formula: see text] is the PG energy. Unanticipated broken-symmetry phases have been detected by a wide variety of techniques in the PG regime, most significantly a finite-Q density-wave (DW) state and a Q = 0 nematic (NE) state. Sublattice-phase-resolved imaging of electronic structure allows the doping and energy dependence of these distinct broken-symmetry states to be visualized simultaneously. Using this approach, we show that even though their reported ordering temperatures T DW and T NE are unrelated to each other, both the DW and NE states always exhibit their maximum spectral intensity at the same energy, and using independent measurements that this is the PG energy [Formula: see text] Moreover, no new energy-gap opening coincides with the appearance of the DW state (which should theoretically open an energy gap on the Fermi surface), while the observed PG opening coincides with the appearance of the NE state (which should theoretically be incapable of opening a Fermi-surface gap). We demonstrate how this perplexing phenomenology of thermal transitions and energy-gap opening at the breaking of two highly distinct symmetries may be understood as the natural consequence of a vestigial nematic state within the pseudogap phase of Bi2Sr2CaCu2O8.


Spin dynamics and field-induced magnetic phase transition in the honeycomb Kitaev magnet alpha-Li2IrO3

PHYSICAL REVIEW B 99 (2019) ARTN 054426

S Choi, S Manni, J Singleton, CV Topping, T Lancaster, SJ Blundell, DT Adroja, V Zapf, P Gegenwart, R Coldea


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

Journal of physics. Condensed matter : an Institute of Physics journal 31 (2019) 013001-

CV Topping, SJ 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.


Unconventional Field-Induced Spin Gap in an S=1/2 Chiral Staggered Chain.

Physical review letters 122 (2019) 057207-

J Liu, S Kittaka, RD Johnson, T Lancaster, J Singleton, T Sakakibara, Y Kohama, J van Tol, A Ardavan, BH Williams, SJ Blundell, ZE Manson, JL Manson, PA Goddard

We investigate the low-temperature magnetic properties of the molecule-based chiral spin chain [Cu(pym)(H_{2}O)_{4}]SiF_{6}·H_{2}O (pym=pyrimidine). Electron-spin resonance, magnetometry and heat capacity measurements reveal the presence of staggered g tensors, a rich low-temperature excitation spectrum, a staggered susceptibility, and a spin gap that opens on the application of a magnetic field. These phenomena are reminiscent of those previously observed in nonchiral staggered chains, which are explicable within the sine-Gordon quantum-field theory. In the present case, however, although the sine-Gordon model accounts well for the form of the temperature dependence of the heat capacity, the size of the gap and its measured linear field dependence do not fit with the sine-Gordon theory as it stands. We propose that the differences arise due to additional terms in the Hamiltonian resulting from the chiral structure of [Cu(pym)(H_{2}O)_{4}]SiF_{6}·H_{2}O, particularly a uniform Dzyaloshinskii-Moriya coupling and a fourfold periodic staggered field.


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.


Magnetic monopole noise.

Nature 571 (2019) 234-239

R Dusad, FKK Kirschner, JC Hoke, BR Roberts, A Eyal, F Flicker, GM Luke, SJ Blundell, JCS Davis

Magnetic monopoles1-3 are hypothetical elementary particles with quantized magnetic charge. In principle, a magnetic monopole can be detected by the quantized jump in magnetic flux that it generates upon passage through a superconducting quantum interference device (SQUID)4. Following the theoretical prediction that emergent magnetic monopoles should exist in several lanthanide pyrochlore magnetic insulators5,6, including Dy2Ti2O7, the SQUID technique has been proposed for their direct detection6. However, this approach has been hindered by the high number density and the generation-recombination fluctuations expected of such thermally generated monopoles. Recently, theoretical advances have enabled the prediction of the spectral density of magnetic-flux noise from monopole generation-recombination fluctuations in these materials7,8. Here we report the development of a SQUID-based flux noise spectrometer and measurements of the frequency and temperature dependence of magnetic-flux noise generated by Dy2Ti2O7 crystals. We detect almost all of the features of magnetic-flux noise predicted for magnetic monopole plasmas7,8, including the existence of intense magnetization noise and its characteristic frequency and temperature dependence. Moreover, comparisons of simulated and measured correlation functions of the magnetic-flux noise indicate that the motions of magnetic charges are strongly correlated. Intriguingly, because the generation-recombination time constant for Dy2Ti2O7 is in the millisecond range, magnetic monopole flux noise amplified by SQUID is audible to humans.


Manipulating quantum materials with quantum light

PHYSICAL REVIEW B 99 (2019) ARTN 085116

M Kiffner, JR Coulthard, F Schlawin, A Ardavan, D Jaksch


Hyperfine interaction of individual atoms on a surface.

Science (New York, N.Y.) 362 (2018) 336-339

P Willke, Y Bae, K Yang, JL Lado, A Ferrón, T Choi, A Ardavan, J Fernández-Rossier, AJ Heinrich, CP Lutz

Taking advantage of nuclear spins for electronic structure analysis, magnetic resonance imaging, and quantum devices hinges on knowledge and control of the surrounding atomic-scale environment. We measured and manipulated the hyperfine interaction of individual iron and titanium atoms placed on a magnesium oxide surface by using spin-polarized scanning tunneling microscopy in combination with single-atom electron spin resonance. Using atom manipulation to move single atoms, we found that the hyperfine interaction strongly depended on the binding configuration of the atom. We could extract atom- and position-dependent information about the electronic ground state, the state mixing with neighboring atoms, and properties of the nuclear spin. Thus, the hyperfine spectrum becomes a powerful probe of the chemical environment of individual atoms and nanostructures.


Static and Fluctuating Magnetic Moments in the Ferroelectric Metal LiOsO3

Proceedings of the 14th International Conference on Muon Spin Rotation, Relaxation and Resonance (μSR2017) Journal of the Physical Society of Japan (2018)

FKK Kirschner, F Lang, FL Pratt, T Lancaster, Y Shi, Y Guo, AT Boothroyd, 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.


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.


Electrically controlled nuclear polarization of individual atoms.

Nature nanotechnology 13 (2018) 1120-1125

K Yang, P Willke, Y Bae, A Ferrón, JL Lado, A Ardavan, J Fernández-Rossier, AJ Heinrich, CP Lutz

Nuclear spins serve as sensitive probes in chemistry1 and materials science2 and are promising candidates for quantum information processing3-6. NMR, the resonant control of nuclear spins, is a powerful tool for probing local magnetic environments in condensed matter systems, which range from magnetic ordering in high-temperature superconductors7,8 and spin liquids9 to quantum magnetism in nanomagnets10,11. Increasing the sensitivity of NMR to the single-atom scale is challenging as it requires a strong polarization of nuclear spins, well in excess of the low polarizations obtained at thermal equilibrium, as well as driving and detecting them individually4,5,12. Strong nuclear spin polarization, known as hyperpolarization, can be achieved through hyperfine coupling with electron spins2. The fundamental mechanism is the conservation of angular momentum: an electron spin flips and a nuclear spin flops. The nuclear hyperpolarization enables applications such as in vivo magnetic resonance imaging using nanoparticles13, and is harnessed for spin-based quantum information processing in quantum dots14 and doped silicon15-17. Here we polarize the nuclear spins of individual copper atoms on a surface using a spin-polarized current in a scanning tunnelling microscope. By employing the electron-nuclear flip-flop hyperfine interaction, the spin angular momentum is transferred from tunnelling electrons to the nucleus of individual Cu atoms. The direction and magnitude of the nuclear polarization is controlled by the direction and amplitude of the current. The nuclear polarization permits the detection of the NMR of individual Cu atoms, which is used to sense the local magnetic environment of the Cu electron spin.


Imaging orbital-selective quasiparticles in the Hund's metal state of FeSe.

Nature materials 17 (2018) 869-874

A Kostin, PO Sprau, A Kreisel, YX Chong, AE Böhmer, PC Canfield, PJ Hirschfeld, BM Andersen, JCS Davis

Strong electronic correlations, emerging from the parent Mott insulator phase, are key to copper-based high-temperature superconductivity. By contrast, the parent phase of an iron-based high-temperature superconductor is never a correlated insulator. However, this distinction may be deceptive because Fe has five actived d orbitals while Cu has only one. In theory, such orbital multiplicity can generate a Hund's metal state, in which alignment of the Fe spins suppresses inter-orbital fluctuations, producing orbitally selective strong correlations. The spectral weights Zm of quasiparticles associated with different Fe orbitals m should then be radically different. Here we use quasiparticle scattering interference resolved by orbital content to explore these predictions in FeSe. Signatures of strong, orbitally selective differences of quasiparticle Zm appear on all detectable bands over a wide energy range. Further, the quasiparticle interference amplitudes reveal that [Formula: see text], consistent with earlier orbital-selective Cooper pairing studies. Thus, orbital-selective strong correlations dominate the parent state of iron-based high-temperature superconductivity in FeSe.


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.

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