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We study the properties of the Dirac states in SiC-graphene and its hole-doped compositions employing angle-resolved photoemission spectroscopy and density functional theory. The symmetry-selective measurements for the Dirac bands reveal their linearly dispersive behavior across the Dirac point which was termed as the anomalous region in earlier studies. No gap is observed even after boron substitution that reduced the carrier concentration significantly from 3.7×10^{13} cm^{-2} in SiC-graphene to 0.8×10^{13} cm^{-2} (5% doping). The anomalies at the Dirac point are attributed to the spectral width arising from the lifetime and momentum broadening in the experiments. The substitution of boron at the graphitic sites leads to a band renormalization and a shift of the Dirac point towards the Fermi level. The internal symmetries appear to be preserved in SiC-graphene even after significant boron substitutions. These results suggest that SiC-graphene is a good platform to realize exotic science as well as advanced technology where the carrier properties like concentration, mobility, etc., can be tuned keeping the Dirac fermionic properties protected.
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We investigate the structural, electronic, and transport properties of substitutional defects in SiC-graphene by means of scanning tunneling microscopy and magnetotransport experiments. Using ion incorporation via ultralow energy ion implantation, the influence of different ion species (boron, nitrogen, and carbon) can directly be compared. While boron and nitrogen atoms lead to an effective doping of the graphene sheet and can reduce or raise the position of the Fermi level, respectively, (12)C(+) carbon ions are used to study possible defect creation by the bombardment. For low-temperature transport, the implantation leads to an increase in resistance and a decrease in mobility in contrast to undoped samples. For undoped samples, we observe in high magnetic fields a positive magnetoresistance that changes to negative for the doped samples, especially for (11)B(+)- and (12)C(+)-ions. We conclude that the conductivity of the graphene sheet is lowered by impurity atoms and especially by lattice defects, because they result in weak localization effects at low temperatures.
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We studied the electronic properties of a high-temperature superconductor in proximity to a ferromagnetic material in a bilayer film of La0.67Sr0.33MnO3 (LSMO)/YBa2Cu3O7 (YBCO). High-quality single-crystalline films of YBCO and LSMO/YBCO were grown epitaxially on an SrTiO3 (001) surface. Magnetization data of the LSMO/YBCO bilayer exhibit ferromagnetic transition at about 255 K, which is much smaller than the Curie temperature of bulk LSMO. Experimental data show the emergence of magnetic anisotropy with cooling, which becomes significantly stronger in the superconducting phase. The onset temperature of diamagnetism is observed at 86 K in the YBCO sample for the out-of-plane magnetization and at 89 K in the in-plane data. Interestingly, the diamagnetism sets in at about 86 K for both magnetization directions in the LSMO/YBCO film despite the presence of the ferromagnetic LSMO layer underneath. Ba 4d and Y 3d core-level spectra show different surface and bulk electronic structures. Surface contribution is reduced significantly in the LSMO/YBCO sample, suggesting enhanced bulk-like behavior due to an enhancement of electron density near the surface arising from charge transfer across the interface. These results reveal an outstanding platform for on-demand tuning of properties without affecting the superconductivity of the system for the exploration of fundamental science and applications in advanced technology.
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Dirac fermions, particles with zero rest mass, are observed in topological materials and are believed to play a key role in the exotic phenomena in fundamental science and the advancement of quantum technology. Most of the topological systems studied so far are weakly correlated systems and the study of their properties in the presence of electron correlation is an interesting emerging area of research, where the electron correlation is expected to enhance the effective mass of the particles. Here, we studied the properties of Dirac bands in a non-symmorphic layered Kondo lattice system, CeAgSb2, employing high-resolution angle-resolved photoemission spectroscopy and first-principles calculations. In addition to the Dirac cones due to non-symmorphic symmetry, this material hosts Dirac fermions in the squarenet layer in the proximity of a strongly correlated Ce layer exhibiting Kondo behavior. Experimental results reveal crossings of the highly dispersive linear bands at the Brillouin zone boundary due to non-symmorphic symmetry. In addition, there are anisotropic Dirac cones constituted by the squarenet Sb 5p states forming a diamond-shaped nodal line. These Dirac bands are linear in a wide energy range with an unusually high slope. Interestingly, near the local Ce 4f bands, these bands exhibit a change in the slope akin to the formation of a 'kink' observed in other materials due to electron-phonon coupling. The emergence of such exotic properties in proximity to strongly correlated electronic states has significant implications in the study of complex quantum materials including unconventional superconductors.
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We investigate the electronic structure of an antiferromagnetic Kondo lattice system CeAgAs2employing hardx-ray photoemission spectroscopy. CeAgAs2, an orthorhombic variant of HfCuSi2structure, exhibits antiferromagnetic ground state, Kondo like resistivity upturn and compensation of magnetic moments at low temperatures. The photoemission spectra obtained at different photon energies suggest termination of the cleaved surface at cis-trans-As layers. The depth-resolved data show significant surface-bulk differences in the As and Ce core level spectra. The As 2pbulk spectrum shows distinct two peaks corresponding to two different As layers. The peak at higher binding energy correspond to cis-trans-As layers and is weakly hybridized with the adjacent Ce layers. The As layers between Ce and Ag-layers possess close to trivalent configuration due to strong hybridization with the neighboring atoms and the corresponding feature appear at lower binding energy. Ce 3dcore level spectra show multiple features reflecting strong Ce-As hybridization and strong correlation. Intensef0peak is observed in the surface spectrum while it is insignificant in the bulk. In addition, we observe a features at binding energy lower than the well-screened feature indicating the presence of additional interactions. This feature becomes more intense in the bulk spectra suggesting it to be a bulk property. Increase in temperature leads to a spectral weight transfer to higher binding energies in the core level spectra and a depletion of spectral intensity at the Fermi level as expected in a Kondo material. These results reveal interesting surface-bulk differences, complex interplay of intra- and inter-layer covalency, and electron correlation in the electronic structure of this novel Kondo lattice system.
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We investigate the properties of excitons in the SiGe inverted quantum huts (IQHs) embedded in Si employing high-resolution x-ray photoemission spectroscopy. Ultra-small Si/Ge IQHs (13.3 nm × 6.6 nm) were grown on a Si buffer layer deposited on a Si (001) substrate using molecular beam epitaxy. We study the behavior of the excitons at different depths of the IQH structures by exposing the desired surfaces via controlled sputtering and annealing processes. The Si and Ge core level spectra show interesting properties at different surfaces; additionally, we discover distinct new features at the lower binding energy side of the Ge 3dpeak. The emergence of these features is attributed to the final state effects arising from core hole screening by the excitons. The properties of these features in the spectra collected at different locations of the IQHs are found significantly different from each other, indicating the local character of the excitons. These results provide a pathway to study the properties of excitons in such quantum structures. The evidence of the local character of the excitons suggests a type I behavior of the system, which is important for the devices for optoelectronic applications, quantum communications, etc.
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We investigate the evolution of the local structural parameters and their implication in unconventional superconductivity of 122 class of materials employing extended x-ray absorption fine structure studies. The spectral functions near the FeK- and AsK-absorption edges of CaFe2As2and its superconducting composition, CaFe1.9Co0.1As2(Tc= 12 K) exhibit evidence of enhancement of Fe contributions near the Fermi level with Co substitution, which becomes more prominent at low temperatures indicating enhanced role of Fe in the electronic properties with doping. As-Fe and Fe-Fe bondlengths derived from the experimental data reveal evolution with temperature across the magneto-structural transition in the parent compound. The evolution of these parameters in Co-doped superconducting composition is similar to its parent compound although no magneto-structural transition is observed in this system. These results reveal an evidence of doping induced evolution to the proximity to critical behavior and/or strong nematic fluctuations which might be important for superconductivity in this system.
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SmB6 has drawn much attention in recent times due to the discovery of anomalies in its ground state properties as well as prediction of topologically protected gapless surface states. Varied theories have been proposed to capture the ground state anomalies. Here, we studied the electronic structure of SmB6 employing density functional theory using different exchange correlation potentials, spin-orbit coupling and electron correlation strength. We discover that a suitable choice of interaction parameters such as spin-orbit coupling, electron correlation strength and exchange interaction within the generalized gradient approximation provides a good description of the spectral functions observed in the angle-resolved photoemission spectroscopy (ARPES) studies. The Fermi surface plots exhibit electron pockets around X-point and hole pockets around ΓX line having dominant Sm 4f character. These observations corroborate well with the recent experimental results involving quantum oscillation measurements, ARPES, etc. In addition to primarily Sm 4f contributions observed at the Fermi level, the results exhibit significantly large contribution from B 2p states compared to weak Sm 5d contributions. This suggests important role of B 2p - Sm 4f hybridization in the exotic physics of this system.
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Employing high resolution hard x-ray photoemission spectroscopy, we investigate the electronic structure of an exotic Fe-based superconductor, CaFe2As2, which exhibits rich temperature pressure phase diagram and dichotomy on achieving superconductivity on application of pressure. The experimental valence band spectra exhibit significant differences for experiments at different surface sensitivities. We discover that the change in angle between light polarization and surface normal leads to similar orbital selective spectral response suggesting requirement of different methodology to probe the surface-bulk differences. Thus, the final state effects of the core level spectroscopy has been exploited to reveal the depth-resolved information. Strong features related to plasmon excitations have been observed in various core level spectra. Ca 2p spectra exhibit evidence of significant hybridization with the conduction electrons, and distinct features corresponding to the surface and bulk electronic structures while As core levels remain unaffected. The depth-resolved Fe 2p spectra at different temperatures exhibit interesting features suggesting structural anomaly may be a bulk property. All these results reveal complexity in the hybridization physics between Fe, As and Ca states presumably leading to exoticity in this material.
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In the series R2PdSi3, Nd2PdSi3 is an anomalous compound in the sense that it exhibits ferromagnetic order unlike other members in this family. The magnetic ordering temperature is also unusually high compared to the expected value for a Nd-based system, assuming 4f localization. Here, we have studied the electronic structure of single crystalline Nd2PdSi3 employing high resolution photoemission spectroscopy and ab initio band structure calculations. Theoretical results obtained for the effective on-site Coulomb energy of 6 eV corroborate well with the experimental valence band spectra. While there is significant Pd 4d-Nd 4f hybridization, the states near the Fermi level are found to be dominated by hybridized Nd 4f-Si 3p states, which is possibly responsible for the ferromagnetism in Nd compound. Nd 3d core level spectrum exhibits multiple features manifesting strong final state effects due to electron correlation, charge transfer and collective excitations. These results serve as one of the rare demonstrations of hybridization of Nd 4f states with the conduction electrons possibly responsible for the exoticity of this compound.
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High-temperature superconductors (HTSs) are important for potential applications and for understanding the origin of strong correlations. Bi2 Sr2 CaCu2 O8+δ (BSCCO), a van der Waals material, offers a platform to probe the physics down to a unit-cell. Guiding the flow of electrons by patterning 2DEGS and oxide heterostructures has brought new functionality and access to new science. Similarly, modifying superconductivity in HTS locally, on a small length scale, is of immense interest for superconducting electronics. A route to modify superconductivity locally by depositing metal on the surface is reported here by transport studies on few unit-cell thick BSCCO. Deposition of chromium (Cr) on the surface over a selected area of BSCCO results in insulating behavior of the underlying region. Cr locally depletes oxygen in CuO2 planes and disrupts the superconductivity in the layers below. This technique of modifying superconductivity is suitable for making sub-micrometer superconducting wires and more complex superconducting devices.
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CaFe2As2 exhibits collapsed tetragonal (cT) structure and varied exotic behaviour under pressure at low temperatures that led to debate on linking the structural changes to its exceptional electronic properties like superconductivity, magnetism, etc. Here, we investigate the electronic structure of CaFe2As2 forming in different structures employing density functional theory. The results indicate that the stability of the cT phase under pressure arises from the enhancement in hybridization induced effects and shift of the energy bands towards lower energies. The Fermi surface centered around Γ point gradually vanishes with the increase in pressure. Consequently, the nesting between the hole and electron Fermi surfaces associated to the spin density wave state disappears indicating a pathway to achieve the proximity to quantum fluctuations. The magnetic moment at the Fe sites diminishes in the cT phase consistent with the magnetic susceptibility results. Notably, the hybridization of Ca 4s states (Ca-layer may be treated as a charge reservoir layer akin to those in cuprate superconductors) is significantly enhanced in the cT phase revealing its relevance in its interesting electronic properties.
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We investigate the electronic structure of a specially prepared highly dense conventional high temperature superconductor, MgB2, employing high resolution photoemission spectroscopy. The spectral evolution close to the Fermi energy is commensurate to BCS descriptions as expected. However, the spectra in the wider energy range reveal the emergence of a pseudogap much above the superconducting transition temperature indicating an apparent departure from the BCS scenario. The energy scale of the pseudogap is comparable to the energy of the [Formula: see text] phonon mode responsible for superconductivity in MgB2 and the pseudogap can be attributed to the effect of electron-phonon coupling on the electronic structure. These results reveal a scenario of the emergence of the superconducting gap within an electron-phonon coupling induced pseudogap and have significant implications in the study of high temperature superconductors.
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The outstanding problem in topological insulators is the bulk metallicity underneath topologically ordered surface states and the appearance of Dirac point far away from the Fermi energy. Enormous efforts are being devoted to get the Dirac point at the Fermi level via exposure to foreign materials so that these materials can be used in technology and realize novel fundamental physics. Ironically, the conclusion of bulk metallicity in the electronic structure is essentially based on the angle resolved photoemission spectroscopy, a highly surface sensitive technique. Here, we employed state-of-the-art hard x-ray photoemission spectroscopy with judiciously chosen experiment geometry to delineate the bulk electronic structure of a topological insulator and a potential thermoelectric material, Bi2Se3. The results exhibit signature of insulating bulk electronic structure with tiny intensities at akin to defect/vacancy induced doped states in the semiconductors. The core level spectra exhibit intense plasmon peak associated to core level excitations manifesting the signature of coupling of electrons to the collective excitations, a possible case of plasmon-phonon coupling. In addition, a new loss feature appear in the core level spectra indicating presence of additional collective excitations in the system.
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Bulk insulators with strong spin orbit coupling exhibit metallic surface states possessing topological order protected by the time reversal symmetry. However, experiments show vulnerability of topological states to aging and impurities. Different studies show contrasting behavior of the Dirac states along with plethora of anomalies, which has become an outstanding problem in material science. Here, we probe the electronic structure of Bi(2)Se(3) employing high resolution photoemission spectroscopy and discover the dependence of the behavior of Dirac particles on surface terminations. The Dirac cone apex appears at different binding energies and exhibits contrasting shift on Bi and Se terminated surfaces with complex time dependence emerging from subtle adsorbed oxygen-surface atom interactions. These results uncover the surface states behavior of real systems and the dichotomy of topological and normal surface states important for device fabrication as well as realization of novel physics such as Majorana Fermions, magnetic monopole, etc.
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We investigate the electronic structure of a complex conventional superconductor, ZrB12 employing high resolution photoemission spectroscopy and ab initio band structure calculations. The experimental valence band spectra could be described reasonably well within the local density approximation. Energy bands close to the Fermi level possess t2g symmetry and the Fermi level is found to be in the proximity of quantum fluctuation regime. The spectral lineshape in the high resolution spectra is complex exhibiting signature of a deviation from Fermi liquid behavior. A dip at the Fermi level emerges above the superconducting transition temperature that gradually grows with the decrease in temperature. The spectral simulation of the dip and spectral lineshape based on a phenomenological self energy suggests finite electron pair lifetime and a pseudogap above the superconducting transition temperature.
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Employing high resolution photoemission spectroscopy, we studied the temperature evolution of the electronic structure of EuFe2As2, a unique pnictide, where antiferromagnetism of the Eu layer survives within the superconducting phase due to 'FeAs' layers, achieved via substitution and/or pressure. High energy and angle resolution helped to reveal the signature of peak-dip features, having significant p orbital character and spin density wave transition induced band folding in the electronic structure. A significant spectral weight redistribution is observed below 20 K manifesting the influence of antiferromagnetic order on the conduction electrons.
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Employing high resolution photoemission spectroscopy, we studied the evolution of the spectral features in rare earth hexaboride single crystals as a function of temperature and 4f binding energy, where the variation of the 4f binding energy is obtained by changing the rare earth element. High energy resolution helped to reveal the distinct features corresponding to the various photoemission final states. Experimental results of CeB(6), a dense Kondo system, exhibit the growth of the features near the Fermi level with the decrease in temperature relative to the uncompensated local moment contributions. The valence band spectra of the antiferromagnetic compounds, PrB(6) and NdB(6), exhibit multiple features-the 4f ionization peaks (poorly screened features) appear at higher binding energies and the features in the vicinity of the Fermi level possessing significant 4f character are due to the well-screened photoemission final states. These results indicate finite hybridization between the 4f and B 2s2p conduction electronic states. Interestingly, the well-screened features in PrB(6) and NdB(6) exhibit unusual enhancement in intensity at low temperature.
Assuntos
Compostos de Boro/química , Césio/química , Elétrons , Neodímio/química , Praseodímio/química , Espectroscopia FotoeletrônicaRESUMO
Kondo systems are usually described by the interaction of the correlation induced local moments with the highly itinerant conduction electrons. Here, we study the role of electron correlations among conduction electrons in the electronic structure of a Kondo lattice compound, Ce2CoSi3, using high resolution photoemission spectroscopy and ab initio band structure calculations, where Co 3d electrons contribute in the conduction band. High energy resolution employed in the measurements helped to reveal the signatures of Ce 4f states derived Kondo resonance features at the Fermi level and the dominance of Co 3d contributions at higher binding energies in the conduction band. The lineshape of the experimental Co 3d band is found to be significantly different from that obtained from the band structure calculations within the local density approximations, LDA. Consideration of electron-electron Coulomb repulsion, U, among Co 3d electrons within the LDA + U method leads to a better representation of experimental results. The signature of an electron correlation induced satellite feature is also observed in the Co 2p core level spectrum. These results clearly demonstrate the importance of the electron correlation among conduction electrons in deriving the microscopic description of such Kondo systems.
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We investigate the temperature evolution of the electronic structure of ferromagnetic CaB6 using ultrahigh resolution photoemission spectroscopy; the electronic structure of paramagnetic LaB6 is used as a reference. High resolution spectra of CaB6 reveal a finite density of states at the Fermi level E(F) at all the temperatures and evidence of impurity induced localized features in the vicinity of E(F), which are absent in the spectra of LaB6. Analysis of the high resolution spectra suggests that disorder in the B sublattice inducing partial localization in the mobile electrons and low electron density at E(F) is important to achieve ferromagnetism in these systems.