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1.
Phys Rev Lett ; 113(21): 216403, 2014 Nov 21.
Artigo em Inglês | MEDLINE | ID: mdl-25479509

RESUMO

We present magnetization, specific heat, and (27)Al NMR investigations on YbFe2Al10 over a wide range in temperature and magnetic field. The magnetic susceptibility at low temperatures is strongly enhanced at weak magnetic fields, accompanied by a ln(T0/T) divergence of the low-T specific heat coefficient in zero field, which indicates a ground state of correlated electrons. From our hard-x-ray photoemission spectroscopy study, the Yb valence at 50 K is evaluated to be 2.38. The system displays valence fluctuating behavior in the low to intermediate temperature range, whereas above 400 K, Yb(3+) carries a full and stable moment, and Fe carries a moment of about 3.1 µB. The enhanced value of the Sommerfeld-Wilson ratio and the dynamic scaling of the spin-lattice relaxation rate divided by T[(27)(1/T1T)] with static susceptibility suggests admixed ferromagnetic correlations. (27)(1/T1T) simultaneously tracks the valence fluctuations from the 4f Yb ions in the high temperature range and field dependent antiferromagnetic correlations among partially Kondo screened Fe 3d moments at low temperature; the latter evolve out of an Yb 4f admixed conduction band.

2.
Phys Rev Lett ; 113(8): 086403, 2014 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-25192112

RESUMO

Pressure dependence of the Ce valence in CeCu(2)Ge(2) has been measured up to 24 GPa at 300 K and to 17 GPa at 18-20 K using x-ray absorption spectroscopy in the partial fluorescence yield. A smooth increase of the Ce valence with pressure is observed across the two superconducting (SC) regions without any noticeable irregularity. The chemical pressure dependence of the Ce valence was also measured in Ce(Cu(1-x)Ni(x))(2)Si(2) at 20 K. A very weak, monotonic increase of the valence with x was observed, without any significant change in the two SC regions. Within experimental uncertainties, our results show no evidence for the valence transition with an abrupt change in the valence state near the SC II region, challenging the valence-fluctuation mediated superconductivity model in these compounds at high pressure and low temperature.

3.
Phys Rev Lett ; 112(11): 117601, 2014 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-24702416

RESUMO

The electronic structure of IrO2 has been investigated using hard x-ray photoelectron spectroscopy and density-functional theory. Excellent agreement is observed between theory and experiment. We show that the electronic structure of IrO2 involves crystal field splitting of the iridium 5d orbitals in a distorted octahedral field. The behavior of IrO2 closely follows the theoretical predictions of Goodenough for conductive rutile-structured oxides [J. B. Goodenough, J. Solid State Chem. 3, 490 (1971).

4.
Nano Lett ; 13(12): 5797-802, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-24228733

RESUMO

The recent focus on topological insulators is due to the scientific interest in the new state of quantum matter as well as the technology potential for a new generation of THz optoelectronics, spintronics and quantum computations. It is important to elucidate the dynamics of the Dirac fermions in the topologically protected surface state. Hence we utilized a novel ultrafast optical pump mid-infrared probe to explore the dynamics of Dirac fermions near the Dirac point. The femtosecond snapshots of the relaxation process were revealed by the ultrafast optics. Specifically, the Dirac fermion-phonon coupling strength in the Dirac cone was found to increase from 0.08 to 0.19 while Dirac fermions were away from the Dirac point into higher energy states. Further, the energy-resolved transient reflectivity spectra disclosed the energy loss rate of Dirac fermions at room temperature was about 1 meV/ps. These results are crucial to the design of Dirac fermion devices.


Assuntos
Nanoestruturas/química , Nanotecnologia , Óptica e Fotônica , Teoria Quântica , Semicondutores , Espectrofotometria Infravermelho
5.
J Synchrotron Radiat ; 20(Pt 2): 266-71, 2013 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-23412483

RESUMO

An X-ray Raman spectrometer for studies of local structures in minerals is discussed. Contrary to widely adopted back-scattering spectrometers using ≤10 keV X-rays, a spectrometer utilizing ~20 keV X-rays and a bent Laue analyzer is proposed. The 20 keV photons penetrate mineral samples much more deeply than 10 keV photons, so that high intensity is obtained owing to an enhancement of the scattering volume. Furthermore, a bent Laue analyzer provides a wide band-pass and a high reflectivity, leading to a much enhanced integrated intensity. A prototype spectrometer has been constructed and performance tests carried out. The oxygen K-edge in SiO(2) glass and crystal (α-quartz) has been measured with energy resolutions of 4 eV (EXAFS mode) and 1.3 eV (XANES mode). Unlike methods previously adopted, it is proposed to determine the pre-edge curve based on a theoretical Compton profile and a Monte Carlo multiple-scattering simulation before extracting EXAFS features. It is shown that the obtained EXAFS features are reproduced fairly well by a cluster model with a minimal set of fitting parameters. The spectrometer and the data processing proposed here are readily applicable to high-pressure studies.

6.
Phys Rev Lett ; 109(4): 046401, 2012 Jul 27.
Artigo em Inglês | MEDLINE | ID: mdl-23006099

RESUMO

We have successfully determined the hitherto unknown sign of the B(4)(4) Stevens crystal-field parameter of the tetragonal heavy-fermion compound CeCu(2)Si(2) using vector q-dependent nonresonant inelastic x-ray scattering experiments at the cerium N(4,5) edge. The observed difference between the two different directions, q∥[100] and q∥[110], is due to the anisotropy of the crystal-field ground state in the (001) plane and is observable only because of the utilization of higher than dipole transitions possible in nonresonant inelastic x-ray scattering. This approach allows us to go beyond the specific limitations of dc magnetic susceptibility, inelastic neutron scattering, and soft x-ray spectroscopy, and provides us with a reliable information about the orbital state of the 4f electrons relevant for the quantitative modeling of the quasiparticles and their interactions in heavy-fermion systems.

7.
J Chem Phys ; 137(24): 244702, 2012 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-23277947

RESUMO

The electronic structure and characteristics of Fe 3d valence states of iron-chalcogenide Fe(1.01)Se superconductors under pressure were probed with x-ray absorption spectroscopy and resonant x-ray emission spectroscopy (RXES). The intensity of the pre-edge peak at ~7112.7 eV of the Fe K-edge x-ray absorption spectrum of Fe(1.01)Se decreases for pressure from 0.5 GPa increased to 6.9 GPa. The satellite line Kß' was reduced in intensity upon applying pressure and became absent for pressure 52 GPa. Fe(1.01)Se shows a small net magnetic moment of Fe(2+), likely arising from strong Fe-Fe spin fluctuations. The 1s3p-RXES spectra of Fe(1.01)Se at pressures 0.5, 6.9, and 52 GPa recorded at the Fe K-edge reveal that unoccupied Fe 3d states exhibit a delocalized character, stemming from hybridization of Fe 3d and 4p orbitals arising from a local distortion around the Fe atom in a tetrahedral site. Application of pressure causes suppression of this on-site Fe 3d-Fe 4p hybridization, and thereby decreases the intensity of the pre-edge feature in the Fe K-edge absorption spectrum of Fe(1.01)Se. Compression enhances spin fluctuations at Fe sites in Fe(1.01)Se and increases the corresponding T(c), through a competition between nearest-neighbor ferromagnetic and next-nearest-neighbor antiferromagnetic superexchange interactions. This result aids our understanding of the physics underlying iron-based superconductors.

8.
Phys Rev Lett ; 104(3): 036103, 2010 Jan 22.
Artigo em Inglês | MEDLINE | ID: mdl-20366662

RESUMO

We demonstrate the charge state of C60 on a Cu(111) surface can be made optimal, i.e., forming C60(3-) as required for superconductivity in bulk alkali-doped C60, purely through interface reconstruction rather than with foreign dopants. We link the origin of the C60(3-) charge state to a reconstructed interface with ordered (4x4) 7-atom vacancy holes in the surface. In contrast, C60 adsorbed on unreconstructed Cu(111) receives a much smaller amount of electrons. Our results illustrate a definitive interface effect that affects the electronic properties of molecule-electrode contact.

9.
J Chem Phys ; 133(15): 154510, 2010 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-20969406

RESUMO

Variations in the electronic structure and structural distortion in multiferroic DyMnO(3) were probed by synchrotron x-ray diffraction, lifetime-broadening-suppressed x-ray absorption spectroscopy (XAS), and ab initio electronic structure calculations. The refined x-ray diffraction data enabled an observation of a diminished local Jahn-Teller distortion of Mn sites within MnO(6) octahedra in DyMnO(3) on applying the hydrostatic pressure. The intensity of the white line in Mn K-edge x-ray absorption spectra of DyMnO(3) progressively increased with the increasing pressure. With the increasing hydrostatic pressure, the absorption threshold of an Mn K-edge spectra of DyMnO(3) shifted toward a greater energy, whereas the pre-edge line slightly shifted to a smaller energy. We provide the spectral evidence for the pressure-induced bandwidth broadening for manganites. The intensity enhancement of the white line in Mn K-edge spectra is attributed to a diminished Jahn-Teller distortion of MnO(6) octahedra in compressed DyMnO(3). A comparison of the pressure-dependent XAS spectra with the ab initio electronic structure calculations and full calculations of multiple scattering using the code FDMNES shows the satisfactory agreement between experimental and calculated Mn K-edge spectra.

10.
J Phys Condens Matter ; 19(17): 176009, 2007 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-21690946

RESUMO

We have investigated the bonding nature and hole-electron Coulomb interaction U in thin C(60) films on Be(0001) surfaces using valence-band and core-level photoemission, inverse photoemission, and near-edge x-ray absorption spectroscopies. The C(60) monolayer had strong covalent bonding with the Be substrate, producing a nearly insulating film, in contrast to a metallic overlayer due to charge transfer observed on many other metallic surfaces. The effect of polarization of surrounding molecules and the image potential decreases the energy gap and U, but the bonding-antibonding contribution increases the gap at the interface. The measured U in thin solid films agrees well with a model calculation using gas-phase values. The deduced hole-electron attraction on the surface is about 0.7 eV larger than the reported hole-hole repulsion determined by Auger spectroscopy. On the basis of the surface-solid difference, the newly estimated value of U for hole-hole correlation places doped C(60) compounds nearer the metallic side of a Mott transition.

11.
Sci Rep ; 5: 10025, 2015 May 18.
Artigo em Inglês | MEDLINE | ID: mdl-25985064

RESUMO

Graphene and its bilayer are two-dimensional systems predicted to show exciting many-body effects near the neutrality point. The ideal tool to investigate spectrum reconstruction effects is angle-resolved photoemission spectroscopy (ARPES) as it probes directly the band structure with information about both energy and momentum. Here we reveal, by studying undoped exfoliated bilayer graphene with ARPES, two essential aspects of its many-body physics: the electron-phonon scattering rate has an anisotropic k-dependence and the type of electronic liquid is non-Fermi liquid. The latter behavior is evident from an observed electron-electron scattering rate that scales linearly with energy from 100 meV to 600 meV and that is associated with the proximity of bilayer graphene to a two-dimensional quantum critical point of competing orders.

12.
Sci Rep ; 5: 17608, 2015 Dec 02.
Artigo em Inglês | MEDLINE | ID: mdl-26626431

RESUMO

We report measurements of the physical properties and electronic structure of the hexagonal compounds Yb2Ni12Pn7 (Pn = P, As) by measuring the electrical resistivity, magnetization, specific heat and partial fluorescence yield x-ray absorption spectroscopy (PFY-XAS). These demonstrate a crossover upon reducing the unit cell volume, from an intermediate valence state in Yb2Ni12As7 to a heavy-fermion paramagnetic state in Yb2Ni12P7, where the Yb is nearly trivalent. Application of pressure to Yb2Ni12P7 suppresses TFL, the temperature below which Fermi liquid behavior is recovered, suggesting the presence of a quantum critical point (QCP) under pressure. However, while there is little change in the Yb valence of Yb2Ni12P7 up to 30 GPa, there is a strong increase for Yb2Ni12As7 under pressure, before a near constant value is reached. These results indicate that any magnetic QCP in this system is well separated from strong valence fluctuations. The pressure dependence of the valence and lattice parameters of Yb2Ni12As7 are compared and at 1 GPa, there is an anomaly in the unit cell volume as well as a change in the slope of the Yb valence, indicating a correlation between structural and electronic changes.

13.
Phys Rev Lett ; 102(2): 026806, 2009 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-19257306

RESUMO

The misfit oxide, Bi2Ba1.3K0.6Co2.1O7.94, made of alternating rocksalt-structured [BiO/BaO] layers and hexagonal CoO2 layers, was studied by angle-resolved photoemission spectroscopy, revealing the electronic structure of a highly strained oxide interface. We found that low-energy states are confined within individual sides of the interface, but scattered by the incommensurate crystal field from the other side. Furthermore, the high strain on the rocksalt layer induces large charge transfer to the CoO2 layer, and a novel effect, the interfacial enhancement of electron-phonon interactions, is discovered.

14.
Phys Rev Lett ; 98(14): 147001, 2007 Apr 06.
Artigo em Inglês | MEDLINE | ID: mdl-17501304

RESUMO

In the present photoemission study of a cuprate superconductor Bi1.74Pb0.38Sr1.88CuO6+delta, we discovered a large scale dispersion of the lowest band, which unexpectedly follows the band structure calculation very well. Similar behavior observed in blue bronze and the Mott insulator Ca2CuO2Cl2 suggests that the origin of hopping-dominated dispersion in an overdoped cuprate might be quite complicated. A giant kink in the dispersion is observed, and the complete self-energy containing all interaction information is extracted for a doped cuprate. These results recovered significant missing pieces in our current understanding of the electronic structure of cuprates.

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