Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 29
Filtrar
Mais filtros










Base de dados
Intervalo de ano de publicação
1.
Nanotechnology ; 33(5)2021 Nov 12.
Artigo em Inglês | MEDLINE | ID: mdl-34670202

RESUMO

Here we report a successful one-step synthesis of vanadium-doped anatase mesocrystals by reactive annealing of NH4TiOF3/PEG2000 mesocrystal precursors with NH4VO3. The formation solid solution Ti1-xVxO2with vanadium content up tox = 25 at% inheriting the structure of mesocrystals is observed for the first time. The doping mechanism via vapor phase transport of vanadium is proposed. The Ti1-xVxO2mesocrystals exhibit improved specific capacity of 175 mAh g-1(compared to 150 mAh g-1for pure anatase phase) and decreased potential gap between charge and discharge processes.

2.
Nat Commun ; 12(1): 1239, 2021 Feb 23.
Artigo em Inglês | MEDLINE | ID: mdl-33623010

RESUMO

One of the main challenges in ultrafast material science is to trigger phase transitions with short pulses of light. Here we show how strain waves, launched by electronic and structural precursor phenomena, determine a coherent macroscopic transformation pathway for the semiconducting-to-metal transition in bistable Ti3O5 nanocrystals. Employing femtosecond powder X-ray diffraction, we measure the lattice deformation in the phase transition as a function of time. We monitor the early intra-cell distortion around the light absorbing metal dimer and the long range deformations governed by acoustic waves propagating from the laser-exposed Ti3O5 surface. We developed a simplified elastic model demonstrating that picosecond switching in nanocrystals happens concomitantly with the propagating acoustic wavefront, several decades faster than thermal processes governed by heat diffusion.

3.
Nat Commun ; 10(1): 2728, 2019 06 21.
Artigo em Inglês | MEDLINE | ID: mdl-31227698

RESUMO

The development of useful structure-function relationships for materials that exhibit correlated nanoscale disorder requires adequately large atomistic models which today are obtained mainly via theoretical simulations. Here, we exploit our recent advances in structure-refinement methodology to demonstrate how such models can be derived directly from simultaneous fitting of 3D diffuse- and total-scattering data, and we use this approach to elucidate the complex nanoscale atomic correlations in the classical relaxor ferroelectric PbMg1/3Nb2/3O3 (PMN). Our results uncover details of ordering of Mg and Nb and reveal a hierarchical structure of polar nanoregions associated with the Pb and Nb displacements. The magnitudes of these displacements and their alignment vary smoothly across the nanoregion boundaries. No spatial correlations were found between the chemical ordering and the polar nanoregions. This work highlights a broadly applicable nanoscale structure-refinement method and provides insights into the structure of PMN that require rethinking its existing contentious models.

4.
J Phys Condens Matter ; 31(17): 175401, 2019 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-30703762

RESUMO

The structure and diffuse scattering in uniaxial relaxor Sr0.6Ba0.4Nb2O6 single crystal have been studied by x-ray diffraction at room temperature. Two different kinds of local ordering with different correlation lengths and different shapes of correlation functions have been revealed. The values of correlation lengths have been determined from analysis of experimental data. These types of orderings are connected with the intrinsic structure of crystal and can promote the appearance of relaxor properties.

5.
J Synchrotron Radiat ; 26(Pt 1): 272-279, 2019 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-30655495

RESUMO

A new diffractometer is now available to the general user community at the ESRF. The new diffractometer is a side station of the high-resolution inelastic X-ray scattering spectrometer on beamline ID28 and is located in the same experimental hutch. Both instruments can be operated simultaneously. The new diffractometer combines a fast and low-noise hybrid pixel detector with a variable diffraction geometry. The beam spot on the sample is 50 µm × 50 µm, where focusing is achieved by a combination of Be lenses and a KB mirror. Wavelengths from 0.5 to 0.8 Šcan be used for the diffraction experiments. The setup is compatible with a variety of sample environments, allowing studies under non-ambient conditions. The diffractometer is optimized to allow a rapid survey of reciprocal space and diffuse scattering for the identification of regions of interest for subsequent inelastic scattering studies, but can also be employed as a fully independent station for structural studies from both powder and single-crystal diffraction experiments. Several software packages for the transformation and visualization of diffraction data are available. An analysis of data collected with the new diffractometer shows that the ID28 side station is a state-of-the-art instrument for structural investigations using diffraction and diffuse scattering experiments.

6.
Science ; 362(6418): 1040-1044, 2018 11 30.
Artigo em Inglês | MEDLINE | ID: mdl-30498124

RESUMO

Cuprates exhibit antiferromagnetic, charge density wave (CDW), and high-temperature superconducting ground states that can be tuned by means of doping and external magnetic fields. However, disorder generated by these tuning methods complicates the interpretation of such experiments. Here, we report a high-resolution inelastic x-ray scattering study of the high-temperature superconductor YBa2Cu3O6.67 under uniaxial stress, and we show that a three-dimensional long-range-ordered CDW state can be induced through pressure along the a axis, in the absence of magnetic fields. A pronounced softening of an optical phonon mode is associated with the CDW transition. The amplitude of the CDW is suppressed below the superconducting transition temperature, indicating competition with superconductivity. The results provide insights into the normal-state properties of cuprates and illustrate the potential of uniaxial-pressure control of competing orders in quantum materials.

7.
Phys Rev Lett ; 119(7): 079903, 2017 Aug 18.
Artigo em Inglês | MEDLINE | ID: mdl-28949658

RESUMO

This corrects the article DOI: 10.1103/PhysRevLett.116.185501.

8.
Phys Rev Lett ; 116(18): 185501, 2016 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-27203332

RESUMO

Comprehensive studies of lattice dynamics in the ferromagnetic semiconductor EuO have been performed by a combination of inelastic x-ray scattering, nuclear inelastic scattering, and ab initio calculations. A remarkably large broadening of the transverse acoustic phonons was discovered at temperatures above and below the Curie temperature T_{C}=69 K. This result indicates a surprisingly strong momentum-dependent spin-phonon coupling induced by the spin dynamics in EuO.

9.
Rev Sci Instrum ; 86(10): 103904, 2015 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-26520968

RESUMO

We present the design, construction, and testing of a straining device compatible with many different synchrotron radiation techniques, in a wide range of experimental environments (including low temperature, high field and ultra-high vacuum). The device has been tested by X-ray diffraction on single crystal samples of quasi-one-dimensional Cs2Mo6Se6 and K2Mo6Se6, in which microscopic strains up to a Δc/c = 0.12% ± 0.01% change in the c lattice parameters have been achieved. We have also used the device in an inelastic X-ray scattering experiment, to probe the strain-dependent speed of sound ν along the c axis. A reduction Δν/ν of up to -3.8% was obtained at a strain of Δc/c = 0.25% in K2Mo6Se6.

10.
J Phys Condens Matter ; 27(32): 325702, 2015 Aug 19.
Artigo em Inglês | MEDLINE | ID: mdl-26214712

RESUMO

X-ray diffraction, specific heat, magnetic susceptibility and inelastic x-ray scattering measurements on the transurarium oxypnictides NpFeAsO and NpFeAsO0.85F0.15 are presented. No superconductivity down to 2 K was observed upon fluorine doping, contrary to the structurally analogous rare-earth pnictides. No modification of the phonon density of states was observed upon doping with fluorine. We discuss our results in light of the latest experimental and theoretical studies on the role of phonons in the superconducting pnictide compounds.

11.
Phys Rev Lett ; 113(2): 025506, 2014 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-25062208

RESUMO

Perfectly crystalline solids are excellent heat conductors. Prominent counterexamples are intermetallic clathrates, guest-host systems with a high potential for thermoelectric applications due to their ultralow thermal conductivities. Our combined experimental and theoretical investigation of the lattice dynamics of a particularly simple binary representative, Ba(8)Si(46), identifies the mechanism responsible for the reduction of lattice thermal conductivity intrinsic to the perfect crystal structure. Above a critical wave vector, the purely harmonic guest-host interaction leads to a drastic transfer of spectral weight to the guest atoms, corresponding to a localization of the propagative phonons.

12.
Phys Rev Lett ; 112(2): 025502, 2014 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-24484025

RESUMO

We measured the density of vibrational states (DOS) and the specific heat of various glassy and crystalline polymorphs of SiO2. The typical (ambient) glass shows a well-known excess of specific heat relative to the typical crystal (α-quartz). This, however, holds when comparing a lower-density glass to a higher-density crystal. For glassy and crystalline polymorphs with matched densities, the DOS of the glass appears as the smoothed counterpart of the DOS of the corresponding crystal; it reveals the same number of the excess states relative to the Debye model, the same number of all states in the low-energy region, and it provides the same specific heat. This shows that glasses have higher specific heat than crystals not due to disorder, but because the typical glass has lower density than the typical crystal.

13.
Nat Mater ; 12(11): 1028-32, 2013 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-23975057

RESUMO

The need for both high electrical conductivity and low thermal conductivity creates a design conflict for thermoelectric systems, leading to the consideration of materials with complicated crystal structures. Rattling of ions in cages results in low thermal conductivity, but understanding the mechanism through studies of the phonon dispersion using momentum-resolved spectroscopy is made difficult by the complexity of the unit cells. We have performed inelastic X-ray and neutron scattering experiments that are in remarkable agreement with our first-principles density-functional calculations of the phonon dispersion for thermoelectric Na(0.8)CoO2, which has a large-period superstructure. We have directly observed an Einstein-like rattling mode at low energy, involving large anharmonic displacements of the sodium ions inside multi-vacancy clusters. These rattling modes suppress the thermal conductivity by a factor of six compared with vacancy-free NaCoO2. Our results will guide the design of the next generation of materials for applications in solid-state refrigerators and power recovery.

14.
Nat Commun ; 4: 2229, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-23892459

RESUMO

Antiferroelectrics are essential ingredients for the widely applied piezoelectric and ferroelectric materials: the most common ferroelectric, lead zirconate titanate is an alloy of the ferroelectric lead titanate and the antiferroelectric lead zirconate. Antiferroelectrics themselves are useful in large digital displacement transducers and energy-storage capacitors. Despite their technological importance, the reason why materials become antiferroelectric has remained allusive since their first discovery. Here we report the results of a study on the lattice dynamics of the antiferroelectric lead zirconate using inelastic and diffuse X-ray scattering techniques and the Brillouin light scattering. The analysis of the results reveals that the antiferroelectric state is a 'missed' incommensurate phase, and that the paraelectric to antiferroelectric phase transition is driven by the softening of a single lattice mode via flexoelectric coupling. These findings resolve the mystery of the origin of antiferroelectricity in lead zirconate and suggest an approach to the treatment of complex phase transitions in ferroics.

15.
J Phys Condens Matter ; 24(43): 435701, 2012 Oct 31.
Artigo em Inglês | MEDLINE | ID: mdl-23032696

RESUMO

The crystal and magnetic structures of the superconducting iron-based chalcogenides Rb(y)Fe(2-x)Se(2) have been studied by means of single-crystal synchrotron x-ray and high-resolution neutron powder diffraction in the temperature range 2-570 K. The ground state of the crystal is an intrinsically phase-separated state with two distinct-by-symmetry phases. The main phase has the iron vacancy ordered √5 × âˆš5 superstructure (I4/m space group) with AFM ordered Fe spins. The minority phase does not have √5 × âˆš5-type of ordering and has a smaller in-plane lattice constant a and larger tetragonal c-axis and can be well described by assuming the parent average vacancy disordered structure (I4/mmm space group) with the refined stoichiometry Rb(0.60(5))(Fe(1.10(5))Se)(2). The minority phase amounts to 8-10% mass fraction. The unit cell volume of the minority phase is 3.2% smaller than the one of the main phase at T = 2 K and has quite different temperature dependence. The minority phase merges with the main vacancy ordered phase on heating above the phase separation temperature T(P) = 475 K. The spatial dimensions of the phase domains strongly increase above T(P) from 1000 to >2500 Å due to the integration of the regions of the main phase that were separated by the second phase at low temperatures. Additional annealing of the crystals at a temperature T = 488 K, close to T(P), for a long time drastically reduces the amount of the minority phase.

16.
Phys Rev Lett ; 109(9): 097603, 2012 Aug 31.
Artigo em Inglês | MEDLINE | ID: mdl-23002887

RESUMO

Complementary diffuse and inelastic synchrotron x-ray scattering measurements of lead zirconate-titanate single crystals with composition near the morphotropic phase boundary (x=0.475) are reported. In the temperature range 293 K

17.
Phys Rev Lett ; 108(4): 045502, 2012 Jan 27.
Artigo em Inglês | MEDLINE | ID: mdl-22400861

RESUMO

We have measured phonon dispersion relations of the high-pressure phase cerium-oC4 (α' phase with the α-uranium crystal structure) at 6.5 GPa by using inelastic x-ray scattering. Pronounced phonon anomalies are observed, which are remarkably similar to those of α-U. First-principles electronic structure calculations reproduce the anomalies and allow us to identify strong electron-phonon coupling as their origin. At the low-pressure end of its stability range, Ce-oC4 is on the verge of a lattice-dynamical instability and possibly a charge density wave. The superconducting transition temperatures of the fcc, oC4, and mC4 phases of Ce have been calculated, and the superconductivity observed experimentally by Wittig and Probst is attributed to the oC4 phase.

18.
Acta Crystallogr A ; 68(Pt 1): 117-23, 2012 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-22186288

RESUMO

The available body of experimental data in terms of the relaxor-specific component of diffuse scattering is critically analysed and a collection of related models is reviewed; the sources of experimental artefacts and consequent failures of modelling efforts are enumerated. Furthermore, it is shown that the widely used concept of polar nanoregions as individual static entities is incompatible with the experimental diffuse scattering results. Based on the synchrotron diffuse scattering three-dimensional data set taken for the prototypical ferroelectric relaxor lead magnesium niobate-lead titanate (PMN-PT), a new parameterization of diffuse scattering in relaxors is presented and a simple phenomenological picture is proposed to explain the unusual properties of the relaxor behaviour. The model assumes a specific slowly changing displacement pattern, which is indirectly controlled by the low-energy acoustic phonons of the system. The model provides a qualitative but rather detailed explanation of temperature, pressure and electric-field dependence of diffuse neutron and X-ray scattering, as well as of the existence of a hierarchy in the relaxation times of these materials.

19.
Phys Rev Lett ; 106(22): 225501, 2011 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-21702612

RESUMO

We compare the atomic dynamics of the glass to that of the relevant crystal. In the spectra of inelastic scattering, the boson peak of the glass appears higher than the transverse acoustic (TA) singularity of the crystal. However, the density of states shows that they have the same number of states. Increasing pressure causes the transformation of the boson peak of the glass towards the TA singularity of the crystal. Once corrected for the difference in the elastic medium, the boson peak matches the TA singularity in energy and height. This suggests the identical nature of the two features.

20.
Phys Rev Lett ; 106(20): 205501, 2011 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-21668242

RESUMO

Achieving comprehensive information on thin film lattice dynamics so far has eluded well established spectroscopic techniques. We demonstrate here the novel application of grazing incidence inelastic x-ray scattering combined with ab initio calculations to determine the complete elastic stiffness tensor, the acoustic and low-energy optic phonon dispersion relations of thin wurtzite indium nitride films. Indium nitride is an especially relevant example, due to the technological interest for optoelectronic and solar cell applications in combination with other group III nitrides.

SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA
...