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1.
Nat Commun ; 14(1): 2658, 2023 May 09.
Article in English | MEDLINE | ID: mdl-37160929

ABSTRACT

Ferromagnetic (FM) order in a two-dimensional kagome layer is predicted to generate a topological Chern insulator without an applied magnetic field. The Chern gap is largest when spin moments point perpendicular to the kagome layer, enabling the capability to switch topological transport properties, such as the quantum anomalous Hall effect, by controlling the spin orientation. In TbMn6Sn6, the uniaxial magnetic anisotropy of the Tb3+ ion is effective at generating the Chern state within the FM Mn kagome layers while a spin-reorientation (SR) transition to easy-plane order above TSR = 310 K provides a mechanism for switching. Here, we use inelastic neutron scattering to provide key insights into the fundamental nature of the SR transition. The observation of two Tb excitations, which are split by the magnetic anisotropy energy, indicates an effective two-state orbital character for the Tb ion, with a uniaxial ground state and an isotropic excited state. The simultaneous observation of both modes below TSR confirms that orbital fluctuations are slow on magnetic and electronic time scales < ps and act as a spatially-random orbital alloy. A thermally-driven critical concentration of isotropic Tb ions triggers the SR transition.

2.
Phys Rev Lett ; 126(1): 017201, 2021 Jan 08.
Article in English | MEDLINE | ID: mdl-33480800

ABSTRACT

We apply neutron spectroscopy to measure the magnetic dynamics in the S=3/2 magnet ß-CaCr_{2}O_{4} (T_{N}=21 K). The low-energy fluctuations, in the ordered state, resemble large-S linear spin waves from the incommensurate ground state. However, at higher energy transfers, these semiclassical and harmonic dynamics are replaced by an energy and momentum broadened continuum of excitations. Applying kinematic constraints required for energy and momentum conservation, sum rules of neutron scattering, and comparison against exact diagonalization calculations, we show that the dynamics at high-energy transfers resemble low-S one-dimensional quantum fluctuations. ß-CaCr_{2}O_{4} represents an example of a magnet at the border between classical Néel and quantum phases, displaying dual characteristics.

3.
Article in English | MEDLINE | ID: mdl-37588000

ABSTRACT

The magnetic ground state of the pyrochlore Yb2GaSbO7 has remained an enigma for nearly a decade. The persistent spin fluctuations observed by muon spin relaxation measurements at low temperatures have not been adequately explained for this material using existing theories for quantum magnetism. Here we report on the synthesis and characterisation of Yb2GaSbO7 to elucidate the central physics at play. Through DC and AC magnetic susceptibility, heat capacity, and neutron scattering experiments, we observe evidence for a dynamical ground state that makes Yb2GaSbO7 a promising candidate for disorder-induced spin-liquid or spin-singlet behaviour. This state is quite fragile, being tuned to a splayed ferromagnet in a modest magnetic field µ0Hc∼1.5T.

4.
J Phys Condens Matter ; 32(37): 374011, 2020 Jun 18.
Article in English | MEDLINE | ID: mdl-32554874

ABSTRACT

Motivated by the presence of an unquenched orbital angular momentum in CoO, a team at Chalk River, including a recently hired research officer Roger Cowley, performed the first inelastic neutron scattering experiments on the classic Mott insulator [Sakurai et al 1968 Phys. Rev. 167 510]. Despite identifying two magnon modes at the zone boundary, the team was unable to parameterise the low energy magnetic excitation spectrum below T N using conventional pseudo-bosonic approaches, instead achieving only qualitative agreement. It would not be for another 40 years that Roger, now at Oxford and motivated by the discovery of the high-T c cuprate superconductors [Bednorz and Muller 1986 Z. Phys. B 64 189], would make another attempt at the parameterisation of the magnetic excitation spectrum that had previously alluded him at the start of his career. Upon his return to CoO, Roger found a system embroiled in controversy, with some of its most fundamental parameters still remaining undetermined. Faced with such a formidable task, Roger performed a series of inelastic neutron scattering experiments in the early 2010s on both CoO and a magnetically dilute structural analogue Mg0.97Co0.03O. These experiments would prove instrumental in the determination of both single-ion [Cowley et al 2013 Phys. Rev. B 88 205117] and cooperative magnetic parameters [Sarte et al 2018 Phys. Rev. B 98 024415] for CoO. Both these sets of parameters would eventually be used in a spin-orbit exciton model [Sarte et al 2019 Phys. Rev. B 100 075143], developed by his longtime friend and collaborator Bill Buyers, to successfully parameterise the complex spectrum that both measured at Chalk River almost 50 years prior. The story of CoO is of one that has come full circle, one filled with both spectacular failures and intermittent, yet profound, little victories.

5.
J Phys Condens Matter ; 32(37): 374012, 2020 Apr 06.
Article in English | MEDLINE | ID: mdl-32252031

ABSTRACT

Materials based on the cubic perovskite unit cell continue to provide the basis for technologically important materials with two notable recent examples being lead-based relaxor piezoelectrics and lead-based organic-inorganic halide photovoltaics. These materials carry considerable disorder, arising from site substitution in relaxors and molecular vibrations in the organic-inorganics, yet much of our understanding of these systems derives from the initial classic work of Prof. Roger A Cowley, who applied both theory and neutron scattering methods while at Chalk River Laboratories to the study of lattice vibrations in SrTiO3. Neutron scattering continues to play a vital role in characterizing lattice vibrations in perovskites owing to the simple cross section and the wide range of energy resolutions achievable with current neutron instrumentation. We discuss the dynamics that drive the phase transitions in the relaxors and organic-inorganic lead-halides in terms of neutron scattering and compare them to those in phase transitions associated with a 'central peak' and also a soft mode. We review some of the past experimental work on these materials and present new data from high-resolution time-of-flight backscattering spectroscopy taken on organic-inorganic perovskites. We will show that the structural transitions in disordered lead-based perovskites are driven by a broad frequency band of excitations.

6.
Eur J Neurol ; 27(5): 825-832, 2020 05.
Article in English | MEDLINE | ID: mdl-32026543

ABSTRACT

BACKGROUND AND PURPOSE: There is no clear consensus among current guidelines on the preferred admission ward [i.e. intensive care unit (ICU) or stroke unit (SU)] for patients with intracerebral hemorrhage. Based on expert opinion, the American Heart Association and European Stroke Organization recommend treatment in neurological/neuroscience ICUs (NICUs) or SUs. The European Stroke Organization guideline states that there are no studies available directly comparing outcomes between ICUs and SUs. METHODS: We performed an observational study comparing outcomes of 10 811 consecutive non-comatose patients with intracerebral hemorrhage according to admission ward [ICUs, SUs and normal wards (NWs)]. Primary outcomes were the modified Rankin Scale score at discharge and intrahospital mortality. An additional analysis compared NICUs with SUs. RESULTS: Treatment outside an SU was associated with higher odds for an unfavorable outcome [ICU vs. SU: odds ratio (OR), 1.27; 95% confidence interval (CI), 1.09-1.46; NW vs. SU: OR, 1.28; 95% CI, 1.08-1.52] and higher odds for intrahospital mortality (ICU vs. SU: OR, 2.11; 95% CI, 1.75-2.55; NW vs. SU: OR, 1.52; 95% CI, 1.23-1.89). A subgroup analysis of severely affected patients treated in dedicated NICUs (vs. SUs) showed that they had a lower risk of a poor outcome (OR, 0.45; 95% CI, 0.26-0.79). CONCLUSIONS: Treatment in SUs was associated with better functional outcome and reduced mortality compared with ICUs and NWs. Our findings support the current guideline recommendations to treat patients with intracerebral hemorrhage in SUs or NICUs and suggest that some patients may further benefit from NICU treatment.


Subject(s)
Cerebral Hemorrhage , Stroke , Cerebral Hemorrhage/etiology , Cerebral Hemorrhage/therapy , Humans , Intensive Care Units , Length of Stay , Stroke/complications , Stroke/therapy , Treatment Outcome
7.
Sci Adv ; 5(3): eaar5066, 2019 Mar.
Article in English | MEDLINE | ID: mdl-30915391

ABSTRACT

Manley et al. (Science Advances, 16 September 2016, p. e1501814) report the splitting of a transverse acoustic phonon branch below T C in the relaxor ferroelectric Pb[(Mg1/3Nb2/3)1-x Ti x ]O3 with x = 0.30 using neutron scattering methods. Manley et al. argue that this splitting occurs because these phonons hybridize with local, harmonic lattice vibrations associated with polar nanoregions. We show that splitting is absent when the measurement is made using a different neutron wavelength, and we suggest an alternative interpretation.

8.
Article in English | MEDLINE | ID: mdl-33655193

ABSTRACT

The organic-inorganic lead-halide perovskites are composed of organic molecules imbedded in an inorganic framework. The compounds with general formula CH3NH3PbX 3 (MAPbX 3) display large photovoltaic efficiencies for halogens X = Cl, Br, and I in a wide variety of sample geometries and preparation methods. The organic cation and inorganic framework are bound by hydrogen bonds that tether the molecules to the halide anions, and this has been suggested to be important to the optoelectronic properties. We have studied the effects of this bonding using time-of-flight neutron spectroscopy to measure the molecular dynamics in CH3NH3PbCl3 (MAPbCl3). Low-energy/high-resolution neutron backscattering reveals thermally activated molecular dynamics with a characteristic temperature of ~95 K. At this same temperature, higher-energy neutron spectroscopy indicates the presence of an anomalous broadening in energy (reduced lifetime) associated with the molecular vibrations. By contrast, neutron powder diffraction shows that a spatially long-range structural phase transitions occurs at 178 K (cubic → tetragonal) and 173 K (tetragonal → orthorhombic). The large difference between these two temperature scales suggests that the molecular and inorganic lattice dynamics in MAPbCl3 are actually decoupled. With the assumption that underlying physical mechanisms do not change with differing halogens in the organic-inorganic perovskites, we speculate that the energy scale most relevant to the photovoltaic properties of the lead-halogen perovskites is set by the lead-halide bond, not by the hydrogen bond.

9.
Phys Rev Mater ; 3(9)2019.
Article in English | MEDLINE | ID: mdl-33062913

ABSTRACT

The acoustic phonons in the organic-inorganic lead halide perovskites have been reported to have anomalously short lifetimes over a large part of the Brillouin zone. The resulting shortened mean free paths of the phonons have been implicated as the origin of the low thermal conductivity. We apply neutron spectroscopy to show that the same acoustic phonon energy linewidth broadening (corresponding to shortened lifetimes) occurs in the fully inorganic CsPbBr3 by comparing the results on the organic-inorganic CH3NH3PbCl3. We investigate the critical dynamics near the three zone boundaries of the cubic P m 3 ¯ m Brillouin zone of CsPbBr3 and find energy and momentum broadened dynamics at momentum points where the Cs-site (A-site) motions contribute to the cross section. Neutron diffraction is used to confirm that both the Cs and Br sites have unusually large thermal displacements with an anisotropy that mirrors the low temperature structural distortions. The presence of an organic molecule is not necessary to disrupt the low-energy acoustic phonons at momentum transfers located away from the zone center in the lead halide perovskites and such damping may be driven by the large displacements or possibly disorder on the A site.

10.
Nat Commun ; 9(1): 4971, 2018 11 26.
Article in English | MEDLINE | ID: mdl-30478378

ABSTRACT

P-type ATPases ubiquitously pump cations across biological membranes to maintain vital ion gradients. Among those, the chimeric K+ uptake system KdpFABC is unique. While ATP hydrolysis is accomplished by the P-type ATPase subunit KdpB, K+ has been assumed to be transported by the channel-like subunit KdpA. A first crystal structure uncovered its overall topology, suggesting such a spatial separation of energizing and transporting units. Here, we report two cryo-EM structures of the 157 kDa, asymmetric KdpFABC complex at 3.7 Å and 4.0 Å resolution in an E1 and an E2 state, respectively. Unexpectedly, the structures suggest a translocation pathway through two half-channels along KdpA and KdpB, uniting the alternating-access mechanism of actively pumping P-type ATPases with the high affinity and selectivity of K+ channels. This way, KdpFABC would function as a true chimeric complex, synergizing the best features of otherwise separately evolved transport mechanisms.


Subject(s)
Cryoelectron Microscopy , Escherichia coli Proteins/metabolism , Potassium/metabolism , Protein Subunits/metabolism , Electron Spin Resonance Spectroscopy , Escherichia coli Proteins/chemistry , Escherichia coli Proteins/ultrastructure , Ion Transport , Protein Conformation , Protein Subunits/chemistry
11.
Phys Rev Lett ; 121(8): 087201, 2018 Aug 24.
Article in English | MEDLINE | ID: mdl-30192563

ABSTRACT

RbFe^{2+}Fe^{3+}F_{6} is an example of a charge ordered antiferromagnet where iron sites, with differing valences, are structurally separated into two interpenetrating sublattices. The low temperature magnetically ordered Fe^{2+} (S=2) and Fe^{3+} (S=5/2) moments form a noncollinear orthogonal structure with the Fe^{3+} site displaying a reduced static ordered moment. Neutron spectroscopy on single crystals finds two distinct spin wave branches with a dominant coupling along the Fe^{3+} chain axis (b axis). High resolution spectroscopic measurements find an intense energy and momentum broadened magnetic band of scattering bracketing a momentum-energy region where two magnon processes are kinematically allowed. These anharmonic excitations are enhanced in this noncollinear magnet owing to the orthogonal spin arrangement.

12.
Phys Rev Lett ; 121(3): 037003, 2018 Jul 20.
Article in English | MEDLINE | ID: mdl-30085774

ABSTRACT

CeCo(In_{0.990}Hg_{0.010})_{5} is a charge doped variant of the d-wave CoCoIn_{5} superconductor with coexistent antiferromagnetic and superconducting transitions occurring at T_{N}=3.4 and T_{c}=1.4 K, respectively. We use neutron diffraction and spectroscopy to show that the magnetic resonant fluctuations present in the parent superconducting phase are replaced by collinear c-axis magnetic order with three-dimensional Ising critical fluctuations. No low-energy transverse spin fluctuations are observable in this doping-induced antiferromagnetic phase and the dynamic resonant spectral weight predominately shifts to the elastic channel. Static (τ>0.2 ns) collinear Ising order is proximate to superconductivity in CeCoIn_{5} and is stabilized through hole doping with Hg.

13.
J Phys Condens Matter ; 30(12): 125703, 2018 03 28.
Article in English | MEDLINE | ID: mdl-29488465

ABSTRACT

The relaxor PbMg1/3Nb2/3O3 (PMN) has received attention due to its potential applications as a piezoelectric when doped with PbTiO3 (PT). Previous results have found that there are two phases existing in the system, one linked to the near-surface regions of the sample, the other in the bulk. However, the exact origin of these two phases is unclear. In this paper, depth dependant analysis results from negative muon implantation experiments are presented. It is shown that the Pb content is constant throughout all depths probed in the sample, but the Mg and Nb content changes in the near-surface region below 100 µm. At an implantation depth of 60 µm, it is found that there is a 25% increase in Mg content, with a simultaneous 5% decrease in Nb content in order to maintain charge neutrality. These results show that the previously observed skin effects in PMN are due to a change in concentration and unit cell.

14.
Phys Rev Mater ; 2(12)2018 Dec.
Article in English | MEDLINE | ID: mdl-38915935

ABSTRACT

Lead halide hybrid perovskites consist of an inorganic framework hosting a molecular cation located in the interstitial space. These compounds have been extensively studied as they have been identified as promising materials for photovoltaic applications with the interaction between the molecular cation and the inorganic framework implicated as influential for the electronic properties. CH3NH3PbCl3 undergoes two structural transitions from a high temperature cubic unit cell to a tetragonal phase at 177 K and then a subsequent orthorhombic transition at 170 K. We have measured the low-frequency lattice dynamics using neutron spectroscopy and observe an energy broadening in the acoustic phonon linewidth towards the high-symmetry point Q X = ( 2 , 1 2 , 0 ) when approaching the transitions. Concomitant with these zone boundary anomalies is a hardening of the entire acoustic phonon branch measured in the q → 0 limit near the (2, 0, 0) Bragg position with decreasing temperature. Measurements of the elastic scattering at the Brillouin zone edges Q X = ( 2 , 1 2 , 0 ) , Q M = ( 3 2 , 1 2 , 0 ) , and Q R = ( 3 2 , 3 2 , 5 2 ) show Bragg peaks appearing below these structural transitions. Based on selection rules of neutron scattering, we suggest that the higher 177 K transition is displacive with a distortion of the local octahedral environment and the lower transition is a rigid tilt transition of the octahedra. We do not observe any critical broadening in energy or momentum, beyond resolution, of these peaks near the transitions. We compare these results to the critical properties reported near the structural transitions in other perovskites and particularly CsPbCl3 [Y. Fujii, S. Hoshino, Y. Yamada, and G. Shirane, Phys. Rev. B 9, 4549 (1974)]. We suggest that the simultaneous onset of static resolution-limited Bragg peaks at the zone boundaries and the changes in acoustic phonon energies near the zone center is evidence of a coupling between the inorganic framework and the molecular cation. The results also highlight the importance of displacive transitions in organic-inorganic hybrid perovskites.

15.
J Phys Condens Matter ; 29(45): 45LT01, 2017 11 15.
Article in English | MEDLINE | ID: mdl-29049030

ABSTRACT

Magnetic monopoles are hypothesised elementary particles connected by Dirac strings that behave like infinitely thin solenoids (Dirac 1931 Proc. R. Soc. A 133 60). Despite decades of searching, free magnetic monopoles and their Dirac strings have eluded experimental detection, although there is substantial evidence for deconfined magnetic monopole quasiparticles in spin ice materials (Castelnovo et al 2008 Nature 326 411). Here we report the detection of a hierarchy of unequally-spaced magnetic excitations via high resolution inelastic neutron spectroscopic measurements on the quantum spin ice candidate [Formula: see text] [Formula: see text] [Formula: see text]. These excitations are well-described by a simple model of monopole pairs bound by a linear potential (Coldea et al Science 327 177) with an effective tension of 0.642(8) K [Formula: see text] at 1.65 K. The success of the linear potential model suggests that these low energy magnetic excitations are direct spectroscopic evidence for the confinement of magnetic monopole quasiparticles in the quantum spin ice candidate [Formula: see text] [Formula: see text] [Formula: see text].

16.
Phys Rev Lett ; 119(25): 257204, 2017 Dec 22.
Article in English | MEDLINE | ID: mdl-29303328

ABSTRACT

CaFe_{2}O_{4} is an anisotropic S=5/2 antiferromagnet with two competing A (↑↑↓↓) and B (↑↓↑↓) magnetic order parameters separated by static antiphase boundaries at low temperatures. Neutron diffraction and bulk susceptibility measurements, show that the spins near these boundaries are weakly correlated and a carry an uncompensated ferromagnetic moment that can be tuned with a magnetic field. Spectroscopic measurements find these spins are bound with excitation energies less than the bulk magnetic spin waves and resemble the spectra from isolated spin clusters. Localized bound orphaned spins separate the two competing magnetic order parameters in CaFe_{2}O_{4}.

17.
J Phys Condens Matter ; 28(45): 453001, 2016 11 16.
Article in English | MEDLINE | ID: mdl-27608752

ABSTRACT

Magnetic oxyselenides have been a topic of research for several decades, firstly in the context of photoconductivity and thermoelectricity owing to their intrinsic semiconducting properties and ability to tune the energy gap through metal ion substitution. More recently, interest in the oxyselenides has experienced a resurgence owing to the possible relation to strongly correlated phenomena given the fact that many oxyselenides share a similar structure to unconventional superconducting pnictides and chalcogenides. The two dimensional nature of many oxyselenide systems also draws an analogy to cuprate physics where a strong interplay between unconventional electronic phases and localised magnetism has been studied for several decades. It is therefore timely to review the physics of the oxyselenides in the context of the broader field of strongly correlated magnetism and electronic phenomena. Here we review the current status and progress in this area of research with the focus on the influence of lanthanides and transition metal ions on the intertwined magnetic and electronic properties of oxyselenides. The emphasis of the review is on the magnetic properties and comparisons are made with iron based pnictide and chalcogenide systems.

18.
Drug Alcohol Depend ; 168: 128-134, 2016 Nov 01.
Article in English | MEDLINE | ID: mdl-27639131

ABSTRACT

BACKGROUND: Overestimations of non-prescribed stimulant use of peers are well documented in the USA and have also been identified as predictive of personal stimulant consumption. This study aimed to examine whether overestimations of peer use and approval of the use are associated with personal use and attitude towards the use of non-prescribed stimulants among European university students. METHOD: The EU funded 'Social Norms Intervention for the prevention of Polydrug usE (SNIPE)' study was conducted in seven European countries. In a web-based questionnaire, 4482 students were asked about their personal use and their attitude towards non-prescribed stimulant use, as well as the perceived peer use and peer attitude. RESULTS: 59% of students thought that the majority of their peers used non-prescribed stimulants more frequently than themselves, and only 4% thought that the use of the majority was lower than their personal use. The perception that the majority of peers had used non-prescribed stimulants at least once was significantly associated with higher odds for personal use of non-prescribed stimulants (OR: 3.30, 95% CI: 2.32-4.71). In addition, the perception that the majority of peers approved of the non-prescribed use of stimulants was associated with a 4.03 (95% CI: 3.35-4.84) times higher likelihood for personal approval. DISCUSSION: European university students generally perceived the non-prescribed use of stimulants of peers to be higher than their personal use. This perception, as well as a perception of higher approval in the peer group, was associated with a higher likelihood of personal non-prescribed stimulant medication use and approval.


Subject(s)
Attitude , Central Nervous System Stimulants/administration & dosage , Peer Group , Social Norms , Students/psychology , Universities , Europe , Female , Humans , Male , Surveys and Questionnaires
19.
Phys Rev Lett ; 117(1): 017201, 2016 Jul 01.
Article in English | MEDLINE | ID: mdl-27419585

ABSTRACT

CaFe_{2}O_{4} is a S=5/2 anisotropic antiferromagnet based upon zig-zag chains having two competing magnetic structures, denoted as the A (↑↑↓↓) and B (↑↓↑↓) phases, which differ by the c-axis stacking of ferromagnetic stripes. We apply neutron scattering to demonstrate that the competing A and B phase order parameters result in magnetic antiphase boundaries along c which freeze on the time scale of ∼1 ns at the onset of magnetic order at 200 K. Using high resolution neutron spectroscopy, we find quantized spin wave levels and measure 9 such excitations localized in regions ∼1-2 c-axis lattice constants in size. We discuss these in the context of solitary magnons predicted to exist in anisotropic systems. The magnetic anisotropy affords both competing A+B orders as well as localization of spin excitations in a classical magnet.

20.
Adv Exp Med Biol ; 876: 215-220, 2016.
Article in English | MEDLINE | ID: mdl-26782215

ABSTRACT

The tumor microenvironment is characterized by hypoxia, acidosis as well as other metabolic and biochemical alterations. Its role in cancer progression is increasingly appreciated especially on invasive capacity and the formation of metastasis. The effect of acidosis on metastasis formation of two rat carcinoma cell lines was studied in the animal model. In order to analyze the pH dependency of different steps of metastasis formation, invasiveness, cell adhesion and migration of AT-1 prostate cancer cells as well as possible underlying cell signaling pathways were studied in vitro. Acidosis significantly increased the formation of lung metastases of both tumor cell lines in vivo. In vitro, extracellular acidosis neither enhanced invasiveness nor affected cell adhesion to a plastic or to an endothelial layer. However, cellular motility was markedly elevated at pH 6.6 and this effect was sustained even when extracellular pH was switched back to pH 7.4. When analyzing the underlying mechanism, a prominent role of ROS in the induction of migration was observed. Signaling through the MAP kinases ERK1/2 and p38 as well as Src family kinases was not involved. Thus, cancer cells in an acidic microenvironment can acquire enhanced motility, which is sustained even if the tumor cells leave their acidic microenvironment e.g. by entering the blood stream. This increase depended on elevated ROS production and may contribute to the augmented formation of metastases of acidosis-primed tumor cells in vivo.


Subject(s)
Acidosis/pathology , Carcinoma 256, Walker/pathology , Animals , Carcinoma 256, Walker/metabolism , Cell Movement , Female , Hydrogen-Ion Concentration , Male , Neoplasm Metastasis , Rats , Reactive Oxygen Species/metabolism , Tumor Microenvironment
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