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1.
Nat Commun ; 13(1): 4132, 2022 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-35840603

RESUMO

Fermi surfaces are essential for predicting, characterizing and controlling the properties of crystalline metals and semiconductors. Angle-resolved photoemission spectroscopy (ARPES) is the only technique directly probing the Fermi surface by measuring the Fermi momenta (kF) from energy- and angular distribution of photoelectrons dislodged by monochromatic light. Existing apparatus is able to determine a number of kF -vectors simultaneously, but direct high-resolution 3D Fermi surface mapping remains problematic. As a result, no such datasets exist, strongly limiting our knowledge about the Fermi surfaces. Here we show that using a simpler instrumentation it is possible to perform 3D-mapping within a very short time interval and with very high resolution. We present the first detailed experimental 3D Fermi surface as well as other experimental results featuring advantages of our technique. In combination with various light sources our methodology and instrumentation offer new opportunities for high-resolution ARPES in the physical and life sciences.

2.
Inorg Chem ; 59(23): 16913-16923, 2020 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-33205960

RESUMO

We present a systematic study of the evolution of structural parameters and electronic correlations as a function of 3d band filling in a single crystal series of BaT2As2 (T = Cr-Cu). The structure trends are discussed in relation to the orbital occupation of the corresponding d elements supported by calculations of the charge density and electron localization function. Analysis of our specific heat data yields the mass enhancement (m*/mb) throughout the series. By combining the structural data with the mass enhancement values, we find that the decrease in m*/mb for n > 5 follows an increase of the crystal field splitting, determined by the progressive distortion of the As-T-As angle from the ideal tetrahedral environment. This study finds a strong interplay between crystal structure, bonding behavior, band filling, and electronic properties.

3.
Phys Rev Lett ; 125(6): 067001, 2020 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-32845654

RESUMO

We report a systematic elastoresistivity study on LaFe_{1-x}Co_{x}AsO single crystals, which have well separated structural and magnetic transition lines. All crystals show a Curie-Weiss-like nematic susceptibility in the tetragonal phase. The extracted nematic temperature is monotonically suppressed upon cobalt doping, and changes sign around the optimal doping level, indicating a possible nematic quantum critical point beneath the superconducting dome. The amplitude of the nematic susceptibility shows a peculiar double-peak feature. This could be explained by a combined effect of different contributions to the nematic susceptibility, which are amplified at separated doping levels of LaFe_{1-x}Co_{x}AsO.

4.
Molecules ; 25(5)2020 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-32120977

RESUMO

Downsizing well-established materials to the nanoscale is a key route to novel functionalities, in particular if different functionalities are merged in hybrid nanomaterials. Hybrid carbon-based hierarchical nanostructures are particularly promising for electrochemical energy storage since they combine benefits of nanosize effects, enhanced electrical conductivity and integrity of bulk materials. We show that endohedral multiwalled carbon nanotubes (CNT) encapsulating high-capacity (here: conversion and alloying) electrode materials have a high potential for use in anode materials for lithium-ion batteries (LIB). There are two essential characteristics of filled CNT relevant for application in electrochemical energy storage: (1) rigid hollow cavities of the CNT provide upper limits for nanoparticles in their inner cavities which are both separated from the fillings of other CNT and protected against degradation. In particular, the CNT shells resist strong volume changes of encapsulates in response to electrochemical cycling, which in conventional conversion and alloying materials hinders application in energy storage devices. (2) Carbon mantles ensure electrical contact to the active material as they are unaffected by potential cracks of the encapsulate and form a stable conductive network in the electrode compound. Our studies confirm that encapsulates are electrochemically active and can achieve full theoretical reversible capacity. The results imply that encapsulating nanostructures inside CNT can provide a route to new high-performance nanocomposite anode materials for LIB.


Assuntos
Técnicas Eletroquímicas/métodos , Íons/química , Lítio/química , Nanotubos de Carbono/química , Cobalto/química , Condutividade Elétrica , Fontes de Energia Elétrica , Eletrodos , Compostos Férricos/química , Compostos de Manganês/química , Microscopia Eletrônica de Varredura , Microscopia Eletrônica de Transmissão , Nanocompostos/química , Nanocompostos/ultraestrutura , Nanotubos de Carbono/ultraestrutura , Óxidos/química , Estanho/química
5.
Sci Rep ; 9(1): 2766, 2019 Feb 26.
Artigo em Inglês | MEDLINE | ID: mdl-30808936

RESUMO

We investigated the structure-property relationship of Co2MnSi Heusler thin films upon the irradiation with He+ ions. The variation of the crystal structure with increasing ion fluence has been probed using nuclear magnetic resonance (NMR) and transmission electron microscopy (TEM), and associated with the corresponding changes of the magnetic behavior. A decrease of both the structural order and the moment in saturation is observed. Specifically, we detect a direct transition from a highly L21-ordered to a fully A2-disordered structure type and quantify the evolution of the A2 structural contribution as a function of ion fluence. Complementary TEM analysis reveals a spatially-resolved distribution of the L21 and A2 phases showing that the A2 disorder starts at the upper part of the films. The structural degradation in turn leads to a decreasing magnetic moment in saturation in response to the increasing fluence.

6.
Sci Rep ; 7(1): 13625, 2017 10 19.
Artigo em Inglês | MEDLINE | ID: mdl-29051613

RESUMO

The ferrimagnetic and high-capacity electrode material Mn3O4 is encapsulated inside multi-walled carbon nanotubes (CNT). We show that the rigid hollow cavities of the CNT enforce size-controlled nanoparticles which are electrochemically active inside the CNT. The ferrimagnetic Mn3O4 filling is switched by electrochemical conversion reaction to antiferromagnetic MnO. The conversion reaction is further exploited for electrochemical energy storage. Our studies confirm that the theoretical reversible capacity of the Mn3O4 filling is fully accessible. Upon reversible cycling, the Mn3O4@CNT nanocomposite reaches a maximum discharge capacity of 461 mA h g-1 at 100 mA g-1 with a capacity retention of 90% after 50 cycles. We attribute the good cycling stability to the hybrid nature of the nanocomposite: (1) Carbon encasements ensure electrical contact to the active material by forming a stable conductive network which is unaffected by potential cracks of the encapsulate. (2) The CNT shells resist strong volume changes of the encapsulate in response to electrochemical cycling, which in conventional (i.e., non-nanocomposite) Mn3O4 hinders the application in energy storage devices. Our results demonstrate that Mn3O4 nanostructures can be successfully grown inside CNT and the resulting nanocomposite can be reversibly converted and exploited for lithium-ion batteries.

7.
J Magn Reson ; 270: 183-186, 2016 09.
Artigo em Inglês | MEDLINE | ID: mdl-27498338

RESUMO

In this work we introduce a new method, which employs commercial piezo-cantilevers, for a ferromagnetic resonance (FMR) detection from thin, nm-size, films. Our setup has an option to rotate the sample in the magnetic field and it operates up to the high microwave frequencies of 160GHz. Using our cantilever based FMR spectrometer we have investigated a set of samples, namely quasi-bulk and 84nm film Co2FeAl0.5Si0.5 samples, 16nm Fe50Ni50 film and 150nm Sr2FeMoO6 film. Low frequency and room temperature test of our setup using 84nm Co2FeAl0.5Si0.5 film yielded a result identical to a standard X-Band spectrometer, namely a single line with quite small linewidth. Our measurements at low temperatures and high frequencies revealed a quite strong FMR response detected in all samples. The FMR spectra share common features, such as the emergence of the second line with an opposite angular dependence, and a drastic increase of the linewidths with increasing microwave frequency. We believe that these findings are results of the complicated dynamics of the magnetization at low temperatures and high frequencies, which we were able to probe using our cantilever based FMR setup.

8.
Sci Rep ; 6: 32462, 2016 08 30.
Artigo em Inglês | MEDLINE | ID: mdl-27571715

RESUMO

The influence of spin-orbit coupling (SOC) on the physical properties of the 5d(2) system Sr2MgOsO6 is probed via a combination of magnetometry, specific heat measurements, elastic and inelastic neutron scattering, and density functional theory calculations. Although a significant degree of frustration is expected, we find that Sr2MgOsO6 orders in a type I antiferromagnetic structure at the remarkably high temperature of 108 K. The measurements presented allow for the first accurate quantification of the size of the magnetic moment in a 5d(2) system of 0.60(2) µB -a significantly reduced moment from the expected value for such a system. Furthermore, significant anisotropy is identified via a spin excitation gap, and we confirm by first principles calculations that SOC not only provides the magnetocrystalline anisotropy, but also plays a crucial role in determining both the ground state magnetic order and the size of the local moment in this compound. Through comparison to Sr2ScOsO6, it is demonstrated that SOC-induced anisotropy has the ability to relieve frustration in 5d(2) systems relative to their 5d(3) counterparts, providing an explanation of the high TN found in Sr2MgOsO6.

9.
Sci Rep ; 6: 28390, 2016 06 22.
Artigo em Inglês | MEDLINE | ID: mdl-27328948

RESUMO

The Hall effect is a powerful tool for investigating carrier type and density. For single-band materials, the Hall coefficient is traditionally expressed simply by , where e is the charge of the carrier, and n is the concentration. However, it is well known that in the critical region near a quantum phase transition, as it was demonstrated for cuprates and heavy fermions, the Hall coefficient exhibits strong temperature and doping dependencies, which can not be described by such a simple expression, and the interpretation of the Hall coefficient for Fe-based superconductors is also problematic. Here, we investigate thin films of Ba(Fe1-xCox)2As2 with compressive and tensile in-plane strain in a wide range of Co doping. Such in-plane strain changes the band structure of the compounds, resulting in various shifts of the whole phase diagram as a function of Co doping. We show that the resultant phase diagrams for different strain states can be mapped onto a single phase diagram with the Hall number. This universal plot is attributed to the critical fluctuations in multiband systems near the antiferromagnetic transition, which may suggest a direct link between magnetic and superconducting properties in the BaFe2As2 system.

10.
Sci Rep ; 5: 16334, 2015 Nov 09.
Artigo em Inglês | MEDLINE | ID: mdl-26548645

RESUMO

Thin film growth of iron chalcogenides by pulsed laser deposition (PLD) is still a delicate issue in terms of simultaneous control of stoichiometry, texture, substrate/film interface properties, and superconducting properties. The high volatility of the constituents sharply limits optimal deposition temperatures to a narrow window and mainly challenges reproducibility for vacuum based methods. In this work we demonstrate the beneficial introduction of a semiconducting FeSe(1-x)Te(x) seed layer for subsequent homoepitaxial growth of superconducting FeSe(1-x)Te(x) thin film on MgO substrates. MgO is one of the most favorable substrates used in superconducting thin film applications, but the controlled growth of iron chalcogenide thin films on MgO has not yet been optimized and is the least understood. The large mismatch between the lattice constants of MgO and FeSe(1-x)Te(x) of about 11% results in thin films with a mixed texture, that prevents further accurate investigations of a correlation between structural and electrical properties of FeSe(1-x)Te(x). Here we present an effective way to significantly improve epitaxial growth of superconducting FeSe(1-x)Te(x) thin films with reproducible high critical temperatures (≥17 K) at reduced deposition temperatures (200 °C-320 °C) on MgO using PLD. This offers a broad scope of various applications.

11.
J Am Chem Soc ; 135(50): 18824-30, 2013 Dec 18.
Artigo em Inglês | MEDLINE | ID: mdl-24246057

RESUMO

The insulating, fully ordered, double perovskite Sr2CoOsO6 undergoes two magnetic phase transitions. The Os(VI) ions order antiferromagnetically with a propagation vector k = (1/2, 1/2, 0) below TN1 = 108 K, while the high-spin Co(II) ions order antiferromagnetically with a propagation vector k = (1/2, 0, 1/2) below TN2 = 70 K. Ordering of the Os(VI) spins is accompanied by a structural distortion from tetragonal I4/m symmetry to monoclinic I2/m symmetry, which reduces the frustration of the face centered cubic lattice of Os(VI) ions. Density functional theory calculations show that the long-range Os-O-Co-O-Os and Co-O-Os-O-Co superexchange interactions are considerably stronger than the shorter Os-O-Co interactions. The poor energetic overlap between the 3d orbitals of Co and the 5d orbitals of Os appears to be responsible for this unusual inversion in the strength of short and long-range superexchange interactions.

12.
Inorg Chem ; 52(24): 14419-27, 2013 Dec 16.
Artigo em Inglês | MEDLINE | ID: mdl-24283501

RESUMO

Superconducting (SC) and non-superconducting (non-SC)Rb(x)Fe(2-y)Se2 crystals were grown using the "self-flux" technique in order to assign the microstructural changes to the onset of superconductivity in complex iron selenides. The crystals were thoroughly characterized by magnetic susceptibility and transport measurements as well as powder X-ray diffraction. Special attention was paid to the comparison of the microstructure of the crystals with and without the superconducting transition by means of transmission electron microscopy (TEM). It is shown that the alternation of ordered and disordered regions on the sample surface and along the c-axis is characteristic for both SC and non-SC materials and therefore does not necessarily represent a trigger of superconductivity. Three types of electron diffraction patterns were found for the superconducting Rb(x)Fe(2-y)Se2 sample, of which one is observed for the first time and originates from alkali metal ordering. Moreover, for the superconducting Rb(x)Fe(2-y)Se2 material a monoclinic distortion with ß âˆ¼ 87° was observed, leading to the space group I2/m. This monoclinic distortion seems to be an attribute of the superconducting material only, whereas in the non-superconducting sample the orthogonality of the crystallographic axes is preserved.

13.
Phys Rev Lett ; 110(1): 017006, 2013 Jan 04.
Artigo em Inglês | MEDLINE | ID: mdl-23383831

RESUMO

Several angle-resolved photoemission spectroscopy (ARPES) studies reveal a poorly nested Fermi surface of LiFeAs, far away from a spin density wave instability, and clear-cut superconducting gap anisotropies. On the other hand a very different, more nested Fermi surface and dissimilar gap anisotropies have been obtained from quasiparticle interference (QPI) data, which were interpreted as arising from intraband scattering within holelike bands. Here we show that this ARPES-QPI paradox is completely resolved by interband scattering between the holelike bands. The resolution follows from an excellent agreement between experimental quasiparticle scattering data and T-matrix QPI calculations (based on experimental band structure data), which allows disentangling interband and intraband scattering processes.

14.
Phys Rev Lett ; 110(6): 066601, 2013 Feb 08.
Artigo em Inglês | MEDLINE | ID: mdl-23432284

RESUMO

Half-metallic ferromagnetism stands for the technologically sought-after metallicity with 100% spin polarization. Electrical transport should, in principle, sensitively probe half-metallic ferromagnetism, since electron-magnon scattering processes are expected to be absent, with clear-cut consequences for the resistivity and the magnetoresistance. Here we present electrical transport data for single-crystalline Co(2)FeSi, a candidate half-metallic ferromagnet Heusler compound. The data reveal a textbooklike exponential suppression of the electron-magnon scattering rate with decreasing temperature which provides strong evidence that this material indeed possesses perfect spin polarization at low temperature. However, the energy scale for thermally activated spin-flip scattering is relatively low (activation gap Δ≈100 K) which has decisive influence on the magnetoresistance and the anomalous Hall effect, which exhibit strong qualitative changes when crossing T≈100 K.

15.
Phys Rev Lett ; 108(12): 127001, 2012 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-22540616

RESUMO

A crucial step in revealing the nature of unconventional superconductivity is to investigate the symmetry of the superconducting order parameter. Scanning tunneling spectroscopy has proven a powerful technique to probe this symmetry by measuring the quasiparticle interference (QPI) which sensitively depends on the superconducting pairing mechanism. A particularly well-suited material to apply this technique is the stoichiometric superconductor LiFeAs as it features clean, charge neutral cleaved surfaces without surface states and a relatively high T(c)∼18 K. Our data reveal that in LiFeAs the quasiparticle scattering is governed by a van Hove singularity at the center of the Brillouin zone which is in stark contrast to other pnictide superconductors where nesting is crucial for both scattering and s(±) superconductivity. Indeed, within a minimal model and using the most elementary order parameters, calculations of the QPI suggest a dominating role of the holelike bands for the quasiparticle scattering. Our theoretical findings do not support the elementary singlet pairing symmetries s(++), s(±), and d wave. This brings to mind that the superconducting pairing mechanism in LiFeAs is based on an unusual pairing symmetry such as an elementary p wave (which provides optimal agreement between the experimental data and QPI simulations) or a more complex order parameter (e.g., s+id wave symmetry).

16.
Sci Technol Adv Mater ; 9(1): 014102, 2008 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-27877928

RESUMO

Spintronic is a multidisciplinary field and a new research area. New materials must be found for satisfying the different types of demands. The search for stable half-metallic ferromagnets and ferromagnetic semiconductors with Curie temperatures higher than room temperature is still a challenge for solid state scientists. A general understanding of how structures are related to properties is a necessary prerequisite for material design. Computational simulations are an important tool for a rational design of new materials. The new developments in this new field are reported from the point of view of material scientists. The development of magnetic Heusler compounds specifically designed as material for spintronic applications has made tremendous progress in the very recent past. Heusler compounds can be made as half-metals, showing a high spin polarization of the conduction electrons of up to 100% in magnetic tunnel junctions. High Curie temperatures were found in Co2-based Heusler compounds with values up to 1120 K in Co2FeSi. The latest results at the time of writing are a tunnelling magnet resistance (TMR) device made from the Co2FeAl0.5Si0.5 Heusler compound and working at room temperature with a (TMR) effect higher than 200%. Good interfaces and a well-ordered compound are the precondition to realize the predicted half-metallic properties. The series Co2FeAl1- x Si x is found to exhibit half-metallic ferromagnetism over a broad range, and it is shown that electron doping stabilizes the gap in the minority states for x=0.5. This might be a reason for the exceptional temperature behaviour of Co2FeAl0.5Si0.5 TMR devices. Using x-ray diffraction (XRD), it was shown conclusively that Co2FeAl crystallizes in the B2 structure whereas Co2FeSi crystallizes in the L21 structure. For the compounds Co2FeGa or Co2FeGe, with Curie temperatures expected higher than 1000 K, the standard XRD technique using laboratory sources cannot be used to easily distinguish between the two structures. For this reason, the EXAFS technique was used to elucidate the structure of these two compounds. Analysis of the data indicated that both compounds crystallize in the L21 structure which makes these two compounds suitable new candidates as materials in magnetic tunnel junctions.

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