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1.
Phys Rev Lett ; 133(4): 046501, 2024 Jul 26.
Artículo en Inglés | MEDLINE | ID: mdl-39121433

RESUMEN

Quasimolecular orbitals in cluster Mott insulators provide a route to tailor exchange interactions, which may yield novel quantum phases of matter. We demonstrate the cluster Mott character of the lacunar spinel GaTa_{4}Se_{8} using resonant inelastic x-ray scattering (RIXS) at the Ta L_{3} edge. Electrons are fully delocalized over Ta_{4} tetrahedra, forming quasimolecular J_{tet}=3/2 moments. The modulation of the RIXS intensity as function of the transferred momentum q allows us to determine the cluster wave function, which depends on competing intracluster hopping terms that mix states with different character. This mixed wave function is decisive for the macroscopic properties since it affects intercluster hopping and exchange interactions and furthermore renormalizes the effective spin-orbit coupling constant. The versatile wave function, tunable via intracluster hopping, opens a new perspective on the large family of lacunar spinels and cluster Mott insulators in general.

2.
Phys Rev Lett ; 129(20): 207201, 2022 Nov 11.
Artículo en Inglés | MEDLINE | ID: mdl-36461990

RESUMEN

Spinons are well known as the elementary excitations of one-dimensional antiferromagnetic chains, but means to realize spinons in higher dimensions is the subject of intense research. Here, we use resonant x-ray scattering to study the layered trimer iridate Ba_{4}Ir_{3}O_{10}, which shows no magnetic order down to 0.2 K. An emergent one-dimensional spinon continuum is observed that can be well described by XXZ spin-1/2 chains with a magnetic exchange of ∼55 meV and a small Ising-like anisotropy. With 2% isovalent Sr doping, magnetic order appears below T_{N}=130 K along with sharper excitations in (Ba_{1-x}Sr_{x})_{4}Ir_{3}O_{10}. Combining our data with exact diagonalization calculations, we find that the frustrated intratrimer interactions effectively reduce the system into decoupled spin chains, the subtle balance of which can be easily tipped by perturbations such as chemical doping. Our results put Ba_{4}Ir_{3}O_{10} between the one-dimensional chain and two-dimensional quantum spin liquid scenarios, illustrating a new way to suppress magnetic order and realize fractional spinons.

3.
Phys Rev Lett ; 122(10): 106401, 2019 Mar 15.
Artículo en Inglés | MEDLINE | ID: mdl-30932648

RESUMEN

The electronic states of many Mott insulators, including iridates, are often conceptualized in terms of localized atomic states such as the famous "J_{eff}=1/2 state." Although orbital hybridization can strongly modify such states and dramatically change the electronic properties of materials, probing this process is highly challenging. In this Letter, we directly detect and quantify the formation of dimer orbitals in an iridate material Ba_{5}AlIr_{2}O_{11} using resonant inelastic x-ray scattering. Sharp peaks corresponding to the excitations of dimer orbitals are observed and analyzed by a combination of density functional theory calculations and theoretical simulations based on an Ir-Ir cluster model. Such partially delocalized dimer states lead to a redefinition of the angular momentum of the electrons and changes in the magnetic and electronic behaviors of the material. We use this to explain the reduction of the observed magnetic moment with respect to predictions based on atomic states. This study opens new directions to study dimerization in a large family of materials, including solids, heterostructures, molecules, and transient states.

4.
Phys Rev Lett ; 118(20): 207202, 2017 May 19.
Artículo en Inglés | MEDLINE | ID: mdl-28581789

RESUMEN

Entanglement of spin and orbital degrees of freedom drives the formation of novel quantum and topological physical states. Here we report resonant inelastic x-ray scattering measurements of the transition metal oxides Ca_{3}LiOsO_{6} and Ba_{2}YOsO_{6}, which reveals a dramatic spitting of the t_{2g} manifold. We invoke an intermediate coupling approach that incorporates both spin-orbit coupling and electron-electron interactions on an even footing and reveal that the ground state of 5d^{3}-based compounds, which has remained elusive in previously applied models, is a novel spin-orbit entangled J=3/2 electronic ground state. This work reveals the hidden diversity of spin-orbit controlled ground states in 5d systems and introduces a new arena in the search for spin-orbit controlled phases of matter.

5.
Phys Rev Lett ; 118(2): 027202, 2017 Jan 13.
Artículo en Inglés | MEDLINE | ID: mdl-28128620

RESUMEN

We use resonant elastic and inelastic x-ray scattering at the Ir-L_{3} edge to study the doping-dependent magnetic order, magnetic excitations, and spin-orbit excitons in the electron-doped bilayer iridate (Sr_{1-x}La_{x})_{3}Ir_{2}O_{7} (0≤x≤0.065). With increasing doping x, the three-dimensional long range antiferromagnetic order is gradually suppressed and evolves into a three-dimensional short range order across the insulator-to-metal transition from x=0 to 0.05, followed by a transition to two-dimensional short range order between x=0.05 and 0.065. Because of the interactions between the J_{eff}=1/2 pseudospins and the emergent itinerant electrons, magnetic excitations undergo damping, anisotropic softening, and gap collapse, accompanied by weakly doping-dependent spin-orbit excitons. Therefore, we conclude that electron doping suppresses the magnetic anisotropy and interlayer couplings and drives (Sr_{1-x}La_{x})_{3}Ir_{2}O_{7} into a correlated metallic state with two-dimensional short range antiferromagnetic order. Strong antiferromagnetic fluctuations of the J_{eff}=1/2 moments persist deep in this correlated metallic state, with the magnon gap strongly suppressed.

6.
Phys Rev Lett ; 114(12): 126401, 2015 Mar 27.
Artículo en Inglés | MEDLINE | ID: mdl-25860761

RESUMEN

We combine resonant inelastic x-ray scattering and model calculations in the Kondo lattice compound YbInCu_{4}, a system characterized by a dramatic increase in Kondo temperature and associated valence fluctuations below a first-order valence transition at T≃42 K. The bulk-sensitive, element-specific, and valence-projected charge excitation spectra reveal an unusual quasigap in the Yb-derived state density which drives an instability of the electronic structure and renormalizes the low-energy effective Hamiltonian at the transition. Our results provide long-sought experimental evidence for a link between temperature-driven changes in the low-energy Kondo scale and the higher-energy electronic structure of this system.

7.
Phys Rev Lett ; 115(3): 036401, 2015 Jul 17.
Artículo en Inglés | MEDLINE | ID: mdl-26230808

RESUMEN

We present evidence that the metal-insulator transition (MIT) in a tensile-strained NdNiO3 (NNO) film is facilitated by a redistribution of electronic density and that it neither requires Ni charge disproportionation nor a symmetry change [U. Staub et al., Phys. Rev. Lett. 88, 126402 (2002); R. Jaramillo et al., Nat. Phys. 10, 304 (2014)]. Given that epitaxial tensile strain in thin NNO films induces preferential occupancy of the e(g) d(x(2)-y(2)) orbital we propose that the larger transfer integral of this orbital state with the O 2p orbital state mediates a redistribution of electronic density from the Ni atom. A decrease in the Ni d(x(2)-y(2)) orbital occupation is directly observed by resonant inelastic x-ray scattering below the MIT temperature. Furthermore, an increase in the Nd charge occupancy is measured by x-ray absorption at the Nd L(3) edge. Both spin-orbit coupling and crystal field effects combine to break the degeneracy of the Nd 5d states, shifting the energy of the Nd e(g) d(x(2)-y(2)) orbit towards the Fermi level, allowing the A site to become an active acceptor during the MIT. This work identifies the relocation of electrons from the Ni 3d to the Nd 5d orbitals across the MIT. We propose that the insulating gap opens between the Ni 3d and O 2p states, resulting from Ni 3d electron localization. The transition seems to be neither a purely Mott-Hubbard transition nor a simple charge transfer.

8.
Phys Rev Lett ; 112(14): 147201, 2014 Apr 11.
Artículo en Inglés | MEDLINE | ID: mdl-24766006

RESUMEN

We report x-ray resonant magnetic scattering and resonant inelastic x-ray scattering studies of epitaxially strained Sr2IrO4 thin films. The films were grown on SrTiO3 and (LaAlO3)0.3(Sr2AlTaO6)0.7 substrates, under slight tensile and compressive strains, respectively. Although the films develop a magnetic structure reminiscent of bulk Sr2IrO4, the magnetic correlations are extremely anisotropic, with in-plane correlation lengths significantly longer than the out-of-plane correlation lengths. In addition, the compressive (tensile) strain serves to suppress (enhance) the magnetic ordering temperature TN, while raising (lowering) the energy of the zone-boundary magnon. Quantum chemical calculations show that the tuning of magnetic energy scales can be understood in terms of strain-induced changes in bond lengths.

9.
Eur J Clin Microbiol Infect Dis ; 33(6): 983-8, 2014 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-24399364

RESUMEN

In this paper, we demonstrate that Fourier transform infrared (FT-IR) spectroscopy is able to discriminate rapidly between uropathogenic Escherichia coli (UPEC) of key lineages with only relatively simple sample preparation. A total of 95 bacteria from six different epidemiologically important multilocus sequence types (ST10, ST69, ST95, ST73, ST127 and ST131) were used in this project and principal component-discriminant function analysis (PC-DFA) of these samples produced clear separate clustering of isolates, based on the ST. Analysis of data using partial least squares-discriminant analysis (PLS-DA), incorporating cross-validation, indicated a high prediction accuracy of 91.19% for ST131. These results suggest that FT-IR spectroscopy could be a useful method for the rapid identification of members of important UPEC STs.


Asunto(s)
Técnicas de Tipificación Bacteriana/métodos , Espectroscopía Infrarroja por Transformada de Fourier/métodos , Escherichia coli Uropatógena/clasificación , Humanos , Escherichia coli Uropatógena/química
10.
Phys Rev Lett ; 111(5): 057202, 2013 Aug 02.
Artículo en Inglés | MEDLINE | ID: mdl-23952439

RESUMEN

We report a combined experimental and theoretical study of the unusual ferromagnetism in the one-dimensional copper-iridium oxide Sr(3)CuIrO(6). Utilizing Ir L(3) edge resonant inelastic x-ray scattering, we reveal a large gap magnetic excitation spectrum. We find that it is caused by an unusual exchange anisotropy generating mechanism, namely, strong ferromagnetic anisotropy arising from antiferromagnetic superexchange, driven by the alternating strong and weak spin-orbit coupling on the 5d Ir and 3d Cu magnetic ions, respectively. From symmetry consideration, this novel mechanism is generally present in systems with edge-sharing Cu(2+)O(4) plaquettes and Ir(4+)O(6) octahedra. Our results point to unusual magnetic behavior to be expected in mixed 3d-5d transition-metal compounds via exchange pathways that are absent in pure 3d or 5d compounds.

11.
Phys Rev Lett ; 110(7): 076402, 2013 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-25166387

RESUMEN

The electronic structure of the honeycomb lattice iridates Na(2)IrO(3) and Li(2)IrO(3) has been investigated using resonant inelastic x-ray scattering (RIXS). Crystal-field-split d-d excitations are resolved in the high-resolution RIXS spectra. In particular, the splitting due to noncubic crystal fields, derived from the splitting of j(eff)=3/2 states, is much smaller than the typical spin-orbit energy scale in iridates, validating the applicability of j(eff) physics in A(2)IrO(3). We also find excitonic enhancement of the particle-hole excitation gap around 0.4 eV, indicating that the nearest-neighbor Coulomb interaction could be large. These findings suggest that both Na(2)IrO(3) and Li(2)IrO(3) can be described as spin-orbit Mott insulators, similar to the square lattice iridate Sr(2)IrO(4).

12.
J Appl Microbiol ; 114(5): 1285-93, 2013 May.
Artículo en Inglés | MEDLINE | ID: mdl-23398275

RESUMEN

AIM: The purpose of this study was to evaluate a commercial antimicrobial formulation, Byotrol™ G32, as a potential coating for impeding biofilm formation on medical devices such as urinary catheters. METHODS AND RESULTS: The antimicrobial activity of Byotrol™ G32 and its individual constituents has been tested on planktonic and biofilm cultures of uropathogenic bacteria. The Byotrol™ G32 formulation was superior with MICs ranging from 3 µg ml(-1) to 15 µg ml(-1) for planktonic cultures and 3-20 µg ml(-1) for biofilms. Furthermore, Byotrol™ G32 was able to remove established biofilms and act as an antibiofilm surface coating. CONCLUSIONS: Byotrol™ G32 displays impressive antimicrobial activity both in suspension and as a coating. Pretreating medical devices with Byotrol™ G32 may significantly impede biofilm formation and prolong the lifetime of the device. SIGNIFICANCE AND IMPACT OF THE STUDY: Medical devices are indispensable in health care. They are, however, a predisposing factor in infection. This research has demonstrated that Byotrol™ G32 reduces bacterial growth and subsequent biofilm formation. Application of Byotrol™ G32 as a medical device coating could have a significant impact on the costs associated with device replacement and patient morbidity and mortality.


Asunto(s)
Antiinfecciosos/farmacología , Compuestos de Benzalconio/farmacología , Biguanidas/farmacología , Biopelículas/efectos de los fármacos , Compuestos de Amonio Cuaternario/farmacología , Escherichia coli/efectos de los fármacos , Klebsiella pneumoniae/efectos de los fármacos , Pruebas de Sensibilidad Microbiana , Pseudomonas aeruginosa/efectos de los fármacos , Catéteres Urinarios/microbiología
13.
Nat Commun ; 14(1): 5018, 2023 Aug 18.
Artículo en Inglés | MEDLINE | ID: mdl-37596328

RESUMEN

Understanding the interplay between the inherent disorder and the correlated fluctuating-spin ground state is a key element in the search for quantum spin liquids. H3LiIr2O6 is considered to be a spin liquid that is proximate to the Kitaev-limit quantum spin liquid. Its ground state shows no magnetic order or spin freezing as expected for the spin liquid state. However, hydrogen zero-point motion and stacking faults are known to be present. The resulting bond disorder has been invoked to explain the existence of unexpected low-energy spin excitations, although data interpretation remains challenging. Here, we use resonant X-ray spectroscopies to map the collective excitations in H3LiIr2O6 and characterize its magnetic state. In the low-temperature correlated state, we reveal a broad bandwidth of magnetic excitations. The central energy and the high-energy tail of the continuum are consistent with expectations for dominant ferromagnetic Kitaev interactions between dynamically fluctuating spins. Furthermore, the absence of a momentum dependence to these excitations are consistent with disorder-induced broken translational invariance. Our low-energy data and the energy and width of the crystal field excitations support an interpretation of H3LiIr2O6 as a disordered topological spin liquid in close proximity to bond-disordered versions of the Kitaev quantum spin liquid.

14.
Phys Rev Lett ; 108(17): 177003, 2012 Apr 27.
Artículo en Inglés | MEDLINE | ID: mdl-22680895

RESUMEN

We used resonant inelastic x-ray scattering to reveal the nature of magnetic interactions in Sr2IrO4, a 5d transition-metal oxide with a spin-orbit entangled ground state and J(eff)=1/2 magnetic moments. The magnon dispersion in Sr2IrO4 is well-described by an antiferromagnetic Heisenberg model with an effective spin one-half on a square lattice, which renders the low-energy effective physics of Sr2IrO4 much akin to that in superconducting cuprates. This point is further supported by the observation of exciton modes in Sr2IrO4, whose dispersion is strongly renormalized by magnons, which can be understood by analogy to hole propagation in the background of antiferromagnetically ordered spins in the cuprates.

15.
Phys Rev Lett ; 109(15): 157402, 2012 Oct 12.
Artículo en Inglés | MEDLINE | ID: mdl-23102367

RESUMEN

Using resonant inelastic x-ray scattering, we observe in the bilayer iridate Sr3Ir2O7, a spin-orbit coupling driven magnetic insulator with a small charge gap, a magnon gap of ≈92 meV for both acoustic and optical branches. This exceptionally large magnon gap exceeds the total magnon bandwidth of ≈70 meV and implies a marked departure from the Heisenberg model, in stark contrast to the case of the single-layer iridate Sr2IrO4. Analyzing the origin of these observations, we find that the giant magnon gap results from bond-directional pseudodipolar interactions that are strongly enhanced near the metal-insulator transition boundary. This suggests that novel magnetism, such as that inspired by the Kitaev model built on the pseudodipolar interactions, may emerge in small charge-gap iridates.

16.
Phys Rev Lett ; 109(15): 157401, 2012 Oct 12.
Artículo en Inglés | MEDLINE | ID: mdl-23102366

RESUMEN

The electronic structure of Sr3CuIrO6, a model system for the 5d Ir ion in an octahedral environment, is studied through a combination of resonant inelastic x-ray scattering and theoretical calculations. Resonant inelastic x-ray scattering spectra at the Ir L3 edge reveal an Ir t(2g) manifold that is split into three levels, in contrast to the expectations of the strong spin-orbit-coupling limit. Effective Hamiltonian and ab inito quantum chemistry calculations find a strikingly large noncubic crystal field splitting comparable to the spin-orbit coupling, which results in a strong mixing of the j(eff)=1/2 and j(eff)=3/2 states and modifies the isotropic wave functions on which many theoretical models are based.

17.
Rev Sci Tech ; 31(2): 619-30, 2012 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-23413737

RESUMEN

This study, published in October 2009 by the World Organisation for Animal Health (OIE), aimed to estimate the essential costs of veterinary prevention systems in sample countries and to develop economic indicators for the veterinary performance evaluation provided by the OIE Tool for the Evaluation of Performance of Veterinary Services (PVS Tool). Full sets of data were collected from seven developing and transition countries. The sources used were literature review, a questionnaire survey and country visits by the core expert team. The total costs of national prevention systems (NPS), net of donor programmes, ranged from 10 million international dollars in Kyrgyzstan to 167 million international dollars in Turkey. These costs are associated with the size of the livestock sector, in veterinary livestock units (VLUs), and national income. It was concluded that NPS cost per VLU provides a meaningful comparative measure of the cost of service provision, varying from 1.92 international dollars in Uganda to 9.40 international dollars in Turkey. The relationship with national income provides estimated indicators of expected NPS costs for other countries. Introduction of quantitative measures to PVS Evaluations would help when assessing the degree of compliance with OIE standards.


Asunto(s)
Enfermedades de los Animales/prevención & control , Crianza de Animales Domésticos/economía , Control de Enfermedades Transmisibles/economía , Países en Desarrollo/economía , Medicina Veterinaria/economía , Zoonosis/prevención & control , Enfermedades de los Animales/economía , Crianza de Animales Domésticos/estadística & datos numéricos , Animales , Control de Enfermedades Transmisibles/métodos , Recolección de Datos/métodos , Bases de Datos como Asunto , Humanos , Ganado , Medicina Veterinaria/métodos , Zoonosis/economía
18.
Nat Commun ; 13(1): 913, 2022 Feb 17.
Artículo en Inglés | MEDLINE | ID: mdl-35177583

RESUMEN

Excitonic insulators are usually considered to form via the condensation of a soft charge mode of bound electron-hole pairs. This, however, presumes that the soft exciton is of spin-singlet character. Early theoretical considerations have also predicted a very distinct scenario, in which the condensation of magnetic excitons results in an antiferromagnetic excitonic insulator state. Here we report resonant inelastic x-ray scattering (RIXS) measurements of Sr3Ir2O7. By isolating the longitudinal component of the spectra, we identify a magnetic mode that is well-defined at the magnetic and structural Brillouin zone centers, but which merges with the electronic continuum in between these high symmetry points and which decays upon heating concurrent with a decrease in the material's resistivity. We show that a bilayer Hubbard model, in which electron-hole pairs are bound by exchange interactions, consistently explains all the electronic and magnetic properties of Sr3Ir2O7 indicating that this material is a realization of the long-predicted antiferromagnetic excitonic insulator phase.

19.
Microbiology (Reading) ; 157(Pt 5): 1290-1299, 2011 May.
Artículo en Inglés | MEDLINE | ID: mdl-21310787

RESUMEN

Salivaricin 9 (Sal9) is a 2560 Da lantibiotic having just 46 % amino acid identity with its closest known homologue, the Streptococcus pyogenes lantibiotic SA-FF22. The Sal9 locus (designated siv) in Streptococcus salivarius strain 9 was partially sequenced and localized to an approximately 170 kb megaplasmid, which also harbours the locus for the lantibiotic salivaricin A4. The entire locus was fully characterized in the draft genome sequence of S. salivarius strain JIM8780 and shown to consist of eight genes, having the following putative functions: sivK, sensor kinase; sivR, response regulator; sivA, Sal9 precursor peptide; sivM, lantibiotic modification enzyme; sivT, ABC transporter involved in the export of Sal9 and concomitant cleavage of its leader peptide; and sivFEG, encoding lantibiotic self-immunity. Intriguingly, in contrast to strain 9, the siv locus was chromosomally located in strain JIM8780--the first lantibiotic locus shown not to be exclusively plasmid-associated in S. salivarius. Sal9-containing extracts specifically induced lantibiotic production in both strain 9 and strain JIM8780, indicating that Sal9 functions as a signal peptide for upregulation of its own biosynthesis. Screening representative strains of three streptococcal species (S. salivarius, S. pyogenes and S. mitis) for sivA indicated that it was present only in S. salivarius, with 12 of 28 tested S. salivarius positive. Since Sal9 was inhibitory to all tested S. pyogenes strains it appears to have potential as an important component of the bacteriocin armoury of S. salivarius probiotics intended to control S. pyogenes infections of the human oral cavity.


Asunto(s)
Antibacterianos/biosíntesis , Bacteriocinas/biosíntesis , Streptococcus/metabolismo , Secuencia de Aminoácidos , Antibacterianos/química , Proteínas Bacterianas/química , Proteínas Bacterianas/genética , Proteínas Bacterianas/metabolismo , Bacteriocinas/química , Bacteriocinas/genética , Datos de Secuencia Molecular , Señales de Clasificación de Proteína , Alineación de Secuencia , Streptococcus/química , Streptococcus/genética
20.
Phys Rev Lett ; 106(18): 187002, 2011 May 06.
Artículo en Inglés | MEDLINE | ID: mdl-21635120

RESUMEN

We have performed photoemission studies of the electronic structure in LiC(6) and KC(8), a nonsuperconducting and a superconducting graphite intercalation compound, respectively. We have found that the charge transfer from the intercalant layers to graphene layers is larger in KC(8) than in LiC(6), opposite of what might be expected from their chemical composition. We have also measured the strength of the electron-phonon interaction on the graphene-derived Fermi surface to carbon derived phonons in both materials and found that it follows a universal trend where the coupling strength and superconductivity monotonically increase with the filling of graphene π(*) states. This correlation suggests that both graphene-derived electrons and graphene-derived phonons are crucial for superconductivity in graphite intercalation compounds.

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