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1.
Nat Commun ; 15(1): 5389, 2024 Jun 25.
Article in English | MEDLINE | ID: mdl-38918440

ABSTRACT

Plasmon polaritons, or plasmons, are coupled oscillations of electrons and electromagnetic fields that can confine the latter into deeply subwavelength scales, enabling novel polaritonic devices. While plasmons have been extensively studied in normal metals or semimetals, they remain largely unexplored in correlated materials. In this paper, we report infrared (IR) nano-imaging of thin flakes of CsV3Sb5, a prototypical layered Kagome metal. We observe propagating plasmon waves in real-space with wavelengths tunable by the flake thickness. From their frequency-momentum dispersion, we infer the out-of-plane dielectric function ϵ c that is generally difficult to obtain in conventional far-field optics, and elucidate signatures of electronic correlations when compared to density functional theory (DFT). We propose correlation effects might have switched the real part of ϵ c from negative to positive values over a wide range of middle-IR frequencies, transforming the surface plasmons into hyperbolic bulk plasmons, and have dramatically suppressed their dissipation.

2.
Nat Commun ; 14(1): 667, 2023 Feb 07.
Article in English | MEDLINE | ID: mdl-36750576

ABSTRACT

The recently discovered kagome superconductors AV3Sb5 (A = K, Rb, Cs) exhibit unusual charge-density-wave (CDW) orders with time-reversal and rotational symmetry breaking. One of the most crucial unresolved issues is identifying the symmetry of the superconductivity that develops inside the CDW phase. Theory predicts a variety of unconventional superconducting symmetries with sign-changing and chiral order parameters. Experimentally, however, superconducting phase information in AV3Sb5 is still lacking. Here we report the impurity effects in CsV3Sb5 using electron irradiation as a phase-sensitive probe of superconductivity. Our magnetic penetration depth measurements reveal that with increasing impurities, an anisotropic fully-gapped state changes to an isotropic full-gap state without passing through a nodal state. Furthermore, transport measurements under pressure show that the double superconducting dome in the pressure-temperature phase diagram survives against sufficient impurities. These results support that CsV3Sb5 is a non-chiral, anisotropic s-wave superconductor with no sign change both at ambient and under pressure.

3.
Sci Rep ; 12(1): 18957, 2022 Nov 08.
Article in English | MEDLINE | ID: mdl-36348085

ABSTRACT

We investigated the doping and temperature evolutions of the optical response of Sr3(Ir1-xMnx)2O7 single crystals with 0 ≤ x ≤ 0.36 by utilizing infrared spectroscopy. Substitution of 3d transition metal Mn ions into Sr3Ir2O7 is expected to induce an insulator-to-metal transition via the decrease in the magnitude of the spin-orbit coupling and the hole doping. In sharp contrast, our data reveal the resilience of the spin-orbit coupling and the incoherent character of the charge transport. Upon Mn substitution, an incoherent in-gap excitation at about 0.25 eV appeared with the decrease in the strength of the optical transitions between the effective total angular momentum Jeff bands of the Ir ions. The resonance energies of the optical transitions between the Jeff bands which are directly proportional to the magnitude of the spin-orbit coupling hardly varied. In addition to these evolutions of the low-energy response, Mn substitution led to the emergence of a distinct high-energy optical excitation at about 1.2 eV which is larger than the resonance energies of the optical transitions between the Jeff bands. This observation indicates that the Mn 3d states are located away from the Ir 5d states in energy and that the large difference in the on-site energies of the transition metal ions is responsible for the incoherent charge transport and the robustness of the spin-orbit coupling. The effect of Mn substitution was also registered in the temperature dependence of the electronic response. The anomaly in the optical response of the parent compound observed at the antiferromagnetic transition temperature is notably suppressed in the Mn-doped compounds despite the persistence of the long-range antiferromagnetic ordering. The suppression of the spin-charge coupling could be related to charge disproportionation of the Ir ions.

4.
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.

5.
Sci Rep ; 10(1): 22340, 2020 Dec 18.
Article in English | MEDLINE | ID: mdl-33339856

ABSTRACT

We report on optical spectroscopic study of the Sr3(Ir1-xRux)2O7 system over a wide doping regime. We find that the changes in the electronic structure occur in the limited range of the concentration of Ru ions where the insulator-metal transition occurs. In the insulating regime, the electronic structure associated with the effective total angular momentum Jeff = 1/2 Mott state remains robust against Ru doping, indicating the localization of the doped holes. Upon entering the metallic regime, the Mott gap collapses and the Drude-like peak with strange metallic character appears. The evolution of the electronic structure registered in the optical data can be explained in terms of a percolative insulator-metal transition. The phonon spectra display anomalous doping evolution of the lineshapes. While the phonon modes of the compounds deep in the insulating and metallic regimes are almost symmetric, those of the semiconducting compound with x = 0.34 in close proximity to the doping-driven insulator-metal transition show a pronounced asymmetry. The temperature evolution of the phonon modes of the x = 0.34 compound reveals the asymmetry is enhanced in the antiferromagnetic state. We discuss roles of the S = 1 spins of the Ru ions and charge excitations for the conspicuous lineshape asymmetry of the x = 0.34 compound.

6.
Phys Rev Lett ; 125(19): 197203, 2020 Nov 06.
Article in English | MEDLINE | ID: mdl-33216570

ABSTRACT

We theoretically predict and experimentally demonstrate a nonthermal pathway to optically enhance superexchange interaction energies in a material based on exciting ligand-to-metal charge-transfer transitions, which introduces lower-order virtual hopping contributions that are absent in the ground state. We demonstrate this effect in the layered ferromagnetic insulator CrSiTe_{3} by exciting Te-to-Cr charge-transfer transitions using ultrashort laser pulses and detecting coherent phonon oscillations that are impulsively generated by superexchange enhancement via magneto-elastic coupling. This mechanism kicks in below the temperature scale where short-range in-plane spin correlations begin to develop and disappears when the excitation energy is tuned away from the charge-transfer resonance, consistent with our predictions.

7.
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.

8.
Phys Rev Lett ; 123(21): 216402, 2019 Nov 22.
Article in English | MEDLINE | ID: mdl-31809181

ABSTRACT

The pseudogap, d-wave superconductivity and electron-boson coupling are three intertwined key ingredients in the phase diagram of the cuprates. Sr_{2}IrO_{4} is a 5d-electron counterpart of the cuprates in which both the pseudogap and a d-wave instability have been observed. Here, we report spectroscopic evidence for the presence of the third key player in electron-doped Sr_{2}IrO_{4}: electron-boson coupling. A kink in nodal dispersion is observed with an energy scale of ∼50 meV. The strength of the kink changes with doping, but the energy scale remains the same. These results provide the first noncuprate platform for exploring the relationship between the pseudogap, d-wave instability, and electron-boson coupling in doped Mott insulators.

9.
Nat Commun ; 10(1): 1654, 2019 04 10.
Article in English | MEDLINE | ID: mdl-30971694

ABSTRACT

Magneto-elastic distortions are commonly detected across magnetic long-range ordering (LRO) transitions. In principle, they are also induced by the magnetic short-range ordering (SRO) that precedes a LRO transition, which contains information about short-range correlations and energetics that are essential for understanding how LRO is established. However these distortions are difficult to resolve because the associated atomic displacements are exceedingly small and do not break symmetry. Here we demonstrate high-multipole nonlinear optical polarimetry as a sensitive and mode selective probe of SRO induced distortions using CrSiTe3 as a testbed. This compound is composed of weakly bonded sheets of nearly isotropic ferromagnetically interacting spins that, in the Heisenberg limit, would individually be impeded from LRO by the Mermin-Wagner theorem. Our results show that CrSiTe3 evades this law via a two-step crossover from two- to three-dimensional magnetic SRO, manifested through two successive and previously undetected totally symmetric distortions above its Curie temperature.

10.
Sci Rep ; 7(1): 10494, 2017 09 05.
Article in English | MEDLINE | ID: mdl-28874789

ABSTRACT

We report on infrared spectroscopy experiments on the electronic response in (Sr1-x La x )2IrO4 (x = 0, 0.021, and 0.067). Our data show that electron doping induced by La substitution leads to an insulator-to-metal transition. The evolution of the electronic structure across the transition reveals the robustness of the strong electronic correlations against the electron doping. The conductivity data of the metallic compound show the signature of the pseudogap that bears close similarity to the analogous studies of the pseudogap in the underdoped cuprates. While the low energy conductivity of the metallic compound is barely frequency dependent, the formation of the pseudogap is revealed by the gradual suppression of the featureless conductivity below a threshold frequency of about 17 meV. The threshold structure develops below about 100 K which is in the vicinity of the onset of the short-range antiferromagnetic order. Our results demonstrate that the electronic correlations play a crucial role in the anomalous charge dynamics in the (Sr1-x La x )2IrO4 system.

11.
Nat Mater ; 16(2): 200-203, 2017 02.
Article in English | MEDLINE | ID: mdl-28092687

ABSTRACT

Layered perovskite iridates realize a rare class of Mott insulators that are predicted to be strongly spin-orbit coupled analogues of the parent state of cuprate high-temperature superconductors. Recent discoveries of pseudogap, magnetic multipolar ordered and possible d-wave superconducting phases in doped Sr2IrO4 have reinforced this analogy among the single layer variants. However, unlike the bilayer cuprates, no electronic instabilities have been reported in the doped bilayer iridate Sr3Ir2O7. Here we show that Sr3Ir2O7 realizes a weak Mott state with no cuprate analogue by using ultrafast time-resolved optical reflectivity to uncover an intimate connection between its insulating gap and antiferromagnetism. However, we detect a subtle charge density wave-like Fermi surface instability in metallic electron doped Sr3Ir2O7 at temperatures (TDW) close to 200 K via the coherent oscillations of its collective modes, which is reminiscent of that observed in cuprates. The absence of any signatures of a new spatial periodicity below TDW from diffraction, scanning tunnelling and photoemission based probes suggests an unconventional and possibly short-ranged nature of this density wave order.

12.
Sci Rep ; 6: 32632, 2016 09 07.
Article in English | MEDLINE | ID: mdl-27599573

ABSTRACT

We report on infrared spectroscopic studies of the electronic response of the (Sr1-xLax)3Ir2O7 system. Our experiments revealed hallmarks of strong electronic correlations in the evolution of the electronic response across the filling-controlled insulator-metal transition. We observed a collapse of the Jeff = 1/2 Mott gap accompanying the transfer of the spectral weight from the high-energy region to the gap region with electron doping. The intraband conductivity at the metallic side of the transition was found to consist of coherent Drude-like and incoherent responses. The sum rule and the extended Drude model analyses further indicated a large mass enhancement. Our results demonstrate a critical role of the electronic correlations in the charge dynamics of the (Sr1-xLax)3Ir2O7 system.

13.
Nat Mater ; 14(6): 577-82, 2015 Jun.
Article in English | MEDLINE | ID: mdl-25915033

ABSTRACT

Negative compressibility is a sign of thermodynamic instability of open or non-equilibrium systems. In quantum materials consisting of multiple mutually coupled subsystems, the compressibility of one subsystem can be negative if it is countered by positive compressibility of the others. Manifestations of this effect have so far been limited to low-dimensional dilute electron systems. Here, we present evidence from angle-resolved photoemission spectroscopy (ARPES) for negative electronic compressibility (NEC) in the quasi-three-dimensional (3D) spin-orbit correlated metal (Sr1-xLax)3Ir2O7. Increased electron filling accompanies an anomalous decrease of the chemical potential, as indicated by the overall movement of the deep valence bands. Such anomaly, suggestive of NEC, is shown to be primarily driven by the lowering in energy of the conduction band as the correlated bandgap reduces. Our finding points to a distinct pathway towards an uncharted territory of NEC featuring bulk correlated metals with unique potential for applications in low-power nanoelectronics and novel metamaterials.

14.
Sci Rep ; 5: 8533, 2015 Feb 23.
Article in English | MEDLINE | ID: mdl-25704850

ABSTRACT

We report on an angle resolved photoemission (ARPES) study of bulk electron-doped perovskite iridate, (Sr(1-x)La(x))3Ir2O7. Fermi surface pockets are observed with a total electron count in keeping with that expected from La substitution. Depending on the energy and polarization of the incident photons, these pockets show up in the form of disconnected "Fermi arcs", reminiscent of those reported recently in surface electron-doped Sr2IrO4. Our observed spectral variation is consistent with the coexistence of an electronic supermodulation with structural distortion in the system.

15.
Phys Rev Lett ; 111(1): 017204, 2013 Jul 05.
Article in English | MEDLINE | ID: mdl-23863025

ABSTRACT

A high-resolution neutron spectroscopic technique is used to measure momentum-resolved magnon lifetimes in the prototypical two- and three-dimensional antiferromagnets Rb(2)MnF(4) and MnF(2), over the full Brillouin zone and a wide range of temperatures. We rederived theories of the lifetime resulting from magnon-magnon scattering, thereby broadening their applicability beyond asymptotically small regions of wave vector and temperature. Corresponding computations, combined with a small contribution reflecting collisions with domain boundaries, yield excellent quantitative agreement with the data. Comprehensive understanding of magnon lifetimes in simple antiferromagnets provides a solid foundation for current research on more complex magnets.

16.
Br J Surg ; 98(5): 652-8, 2011 May.
Article in English | MEDLINE | ID: mdl-21412997

ABSTRACT

BACKGROUND: The aim was to develop a multivariable risk prediction model for 30-day mortality following elective abdominal aortic aneurysm (AAA) repair. METHODS: Data collected prospectively on 2765 consecutive patients undergoing elective open and endovascular AAA repair from September 1999 to October 2009 in the North West of England were split randomly into development (1936 patients) and validation (829) data sets. Logistic regression analysis was undertaken to identify risk factors for 30-day mortality. RESULTS: Ninety-eight deaths (5·1 per cent) were recorded in the development data set. Variables associated with 30-day mortality included: increasing age (P = 0·005), female sex (P = 0·002), diabetes (P = 0·029), raised serum creatinine level (P = 0·006), respiratory disease (P = 0·031), antiplatelet medication (P < 0·001) and open surgery (P = 0·002). The area under the receiver operating characteristic (ROC) curve for predicted probability of 30-day mortality in the development and validation data sets was 0·73 and 0·70 respectively. Observed versus expected 30-day mortality was 3·2 versus 2·0 per cent (P = 0·272) in low-risk, 6·1 versus 5·1 per cent (P = 0·671) in medium-risk and 11·1 versus 10·7 per cent (P = 0·879) in high-risk patients. CONCLUSION: This multivariable model for predicting 30-day mortality following elective AAA repair can be used clinically to calculate patient-specific risk and is useful for case-mix adjustment. The model predicted well across all risk groups in the validation data set.


Subject(s)
Aortic Aneurysm, Abdominal/surgery , Elective Surgical Procedures/mortality , Adult , Aged , Aortic Aneurysm, Abdominal/mortality , England/epidemiology , Epidemiologic Methods , Female , Humans , Male , Middle Aged
17.
Ultramicroscopy ; 100(3-4): 211-6, 2004 Aug.
Article in English | MEDLINE | ID: mdl-15231312

ABSTRACT

We measured the desorption of explosive trinitrotoluene (TNT), pentaerythritol tetranitrate (PETN), and hexahydro-1,3,5-triazine (RDX) vapors from piezoresistive silicon microcantilevers under ambient air. Depending on the amount of vapor loaded on the cantilever, TNT desorption took a few minutes to tens of minutes (for nanogram quantities). On the other hand, no significant loss of PETN or RDX was observed after many hours. We also measured desorption of common "nonexplosive" compounds (water, acetone, and ethyl alcohol) and observed that desorption was too fast to be measured. There is a good correlation between the desorption time and the melting point (or the vapor pressure) of a particular substance. In principle, this method can be used to measure desorption rates of various substances from cantilever surfaces.

18.
Toxicol Appl Pharmacol ; 177(3): 208-18, 2001 Dec 15.
Article in English | MEDLINE | ID: mdl-11749120

ABSTRACT

A number of methods have been developed to assess the impact of a xenobiotic on the various components of the immune system. For risk analysis, it is necessary to determine what degree of chemically induced immune perturbation translates into altered host resistance. Natural killer (NK) cells play a pivotal role in the innate immune system with the ability to lyse cells infected with intracellular pathogens and certain tumors without previous exposure to the antigen. Spontaneous NK activity in B6C3F1 mice could be incrementally and consistently decreased by 20 to > or =80% by the intravenous administration of a range of dilutions of anti-asialo GM1 (AAGM1) antibody. The decrease in spontaneous NK activity following a single iv administration of AAGM1 antibody persisted for up to approximately 3 weeks when the initial suppression (e.g., 24 h after AAGM1 antibody injection) was almost 100%. Treatment with AAGM1, however, did not appear to perturb the function of other immune cells, based on results of the plaque assay, the mixed lymphocyte response, the cytotoxic T lymphocyte assay, the reticuloendothelial system clearance of sRBC assay, and the Streptococcus pneumoniae host resistance assay. Following a > or =80% decrease in spontaneous NK activity in mice, challenge with > or =1 x 10(3) B16F10 melanoma cells resulted in an increase in tumor burden based on the number of lung nodules. However, following challenge with 1 x 10(5) melanoma cells, a significant increase in tumor burden in mice was not observed until spontaneous NK activity had been decreased by > or =50-60%. Altered host resistance is a function not only of the magnitude of the decrease in NK activity but also of the magnitude of the challenge to the host.


Subject(s)
Immunosuppression Therapy , Killer Cells, Natural/immunology , Animals , Antibodies/pharmacology , Body Weight/drug effects , Cell Count , Cells, Cultured , Crosses, Genetic , Cytotoxicity Tests, Immunologic , Dose-Response Relationship, Immunologic , Erythrocytes/immunology , G(M1) Ganglioside/antagonists & inhibitors , G(M1) Ganglioside/immunology , Immunocompromised Host/immunology , Immunosuppressive Agents/pharmacology , Killer Cells, Natural/cytology , Killer Cells, Natural/drug effects , Melanoma/immunology , Melanoma/pathology , Mice , Mice, Inbred C3H , Mice, Inbred C57BL , Neoplasm Transplantation/immunology , Organ Size/drug effects , Spleen/cytology , Spleen/immunology , Streptococcus pneumoniae/immunology , Streptococcus pneumoniae/pathogenicity , T-Lymphocytes/cytology , T-Lymphocytes/immunology , Xenograft Model Antitumor Assays
19.
Am J Med Qual ; 16(5): 174-80, 2001.
Article in English | MEDLINE | ID: mdl-11591017

ABSTRACT

Despite the rapid growth in pediatric hospitalist services, there is little empiric information about the impact of pediatric hospitalists. This study compared process and outcome variables related to the inpatient care of 182 pediatric patients, half of whom were cared for by hospitalists and half by their primary care providers (PCP). Results indicated that, while hospitalists cared for patients of substantially lower socioeconomic status, they delivered care more economically for patients with asthma, with no significant differences in rates of return to the emergency room or rehospitalizations. Children in both services demonstrated equivalent levels of returning to their PCP for follow-up visits and were in equally good health 1 month after discharge. Additionally, no negative impact was evident on patient satisfaction at discharge; in fact, the hospitalists' patients were more satisfied with aspects of their care. Hospitalists may, therefore, provide a vital service by ensuring quality inpatient care for low-income children.


Subject(s)
Hospitalists , Outcome and Process Assessment, Health Care , Pediatrics , Physicians, Family , Analysis of Variance , Chi-Square Distribution , Child, Preschool , Female , Hospitalists/economics , Hospitalists/standards , Humans , Interviews as Topic , Male , Patient Satisfaction , Physicians, Family/economics , Physicians, Family/standards , Poverty , Prospective Studies , Socioeconomic Factors , Surveys and Questionnaires , Workforce
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