Preparation, Characterization and electronic structure of Ti-doped Bi2_2Se3_3

We report the preparation of high-quality single crystal of Bi$_2$Se$_3$, a well-known topological insulator and its Ti-doped compositions using Bridgeman technique. Prepared single crystals were characterized by x-ray diffraction (XRD) to check the crystalline structure and energy dispersive analysis of x-rays for composition analysis. The XRD data of Ti-doped compounds show a small shift with respect to normal Bi$_2$Se$_3$ indicating changes in the lattice parameters while the structure type remained unchanged; this also establishes that Ti goes to the intended substitution sites. All the above analysis establishes successful preparation of these crystals with high quality using Bridgman technique. We carried out x-ray photo-emission spectroscopy to study the composition via investigating the core level spectra. Bi$_2$Se$_3$ spectra exhibit sharp and distinct features for the core levels and absence of impurity features. The core level spectra of the Ti-doped sample exhibit distinct signal due to Ti core levels. The analysis of the spectral features reveal signature of plasmon excitation and final state satellites; a signature of finite electron correlation effect in the electronic structure.Comment: Proceedings of DAE SSPS 201

Layer-resolved electronic behavior in a Kondo lattice system, CeAgAs2

We investigate the electronic structure of an antiferromagnetic Kondo lattice system CeAgAs2 employing hard x-ray photoemission spectroscopy. CeAgAs2, an orthorhombic variant of HfCuSi2 structure, 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 2p bulk 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 3d core level spectra show multiple features reflecting strong Ce-As hybridization and strong correlation. Intense f0 peak 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

Complexity in the hybridization physics revealed by depth-resolved photoemission spectroscopy of single crystalline novel Kondo lattice systems, CeCuX2_2 (X = As/Sb)

We investigate the electronic structure of a novel Kondo lattice system CeCuX2 (X = As/Sb) employing high resolution depth-resolved photoemission spectroscopy of high quality single crystalline materials. CeCuSb2 and CeCuAs2 represent different regimes of the Doniach phase diagram exhibiting Kondo-like transport properties and CeCuSb2 is antiferromagnetic (TN ~ 6.9 K) while CeCuAs$_2$ does not show long-range magnetic order down to the lowest temperature studied. In this study, samples were cleaved in ultrahigh vacuum before the photoemission measurements and the spectra at different surface sensitivity establish the pnictogen layer having squarenet structure as the terminated surface which is weakly bound to the other layers. Cu 2p and As 2p spectra show spin-orbit split sharp peaks along with features due to plasmon excitations. Ce 3d spectra exhibit multiple features due to the hybridization of the Ce 4f/5d states with the valence states. While overall lineshape of the bulk spectral functions look similar in both the cases, the surface spectra are very different; the surface-bulk difference is significantly weaker in CeCuAs2 compared to that observed in CeCuSb2. A distinct low binding energy peak is observed in the Ce 3d spectra akin to the scenario observed in cuprates and manganites due to the Zhang-Rice singlets and/or high degree of itineracy of the conduction holes. The valence band spectra of CeCuSb$_2$ manifest highly metallic phase. In CeCuAs2, intensity at the Fermi level is significantly small suggesting a pseudogap-type behavior. These results bring out an interesting scenario emphasizing the importance and subtlety of hybridization physics underlying the exoticity of this novel Kondo system

Electronic structure of a Kondo lattice system CeCuAs2_2

We study the electronic properties of a Ce-based Kondo material, CeCuAs$_2$ employing high-resolution hard x-ray photoemission spectroscopy. The measurements were done with different photon energies to probe the surface-bulk differences of the electronic structure. Experimental results show significant difference in the hybridization physics for the surface and bulk electronic structures indicating different Ce valency at the surface compared to the bulk. Surface termination appears to play an important role in the correlation physics of this system. In addition, the experimental spectra show loss features due to plasmon excitations. These results bring out complexity of this novel Kondo lattice system that does not show magnetic order down to the lowest temperature studied and have significantly different surface-bulk properties

Giant spectral renormalization and complex hybridization physics in the Kondo lattice system CeCuSb2_2

We investigate the electronic structure of a Kondo lattice system, CeCuSb$_2$ exhibiting significant mass enhancement and Kondo-type behavior. We observe multiple features in the hard x-ray photoemission spectra of Ce core levels due to strong final-state effects. The depth-resolved data exhibit a significant change in relative intensity of the features with the surface sensitivity of the probe. The extracted surface and bulk spectral functions are different and exhibit a Kondo-like feature at higher binding energies in addition to the well and poorly screened features. The core-level spectra of Sb exhibit huge and complex changes as a function of the surface sensitivity of the technique. The analysis of the experimental data suggests that the two nonequivalent Sb sites possess different electronic structures and in each category, the Sb layers close to the surface are different from the bulk ones. An increase in temperature influences the Ce-Sb hybridization significantly. The plasmon–excitation-induced loss features are also observed in all core-level spectra. All these results reveal the importance of Ce-Sb hybridizations and indicate that the complex renormalization of Ce-Sb hybridization may be the reason for the exotic electronic properties of this system

Layer-resolved electronic behavior in a Kondo lattice system, CeAgAs2_2

We investigate the electronic structure of an antiferromagnetic Kondo lattice system CeAgAs$_2$ employing hard x-ray photoemission spectroscopy. CeAgAs$_2$, an orthorhombic variant of HfCuSi$_2$ structure, 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 2p bulk 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 3d core level spectra show multiple features reflecting strong Ce-As hybridization and strong correlation. Intense f$_0$ peak 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

Emergence of well-screened states in a superconducting material of the CaFe2As2CaFe_{2}As_{2} family

Coupling among conduction electrons (e.g., Zhang-Rice singlet) are often manifested in the core level spectra of exotic materials such as cuprate superconductors, manganites, etc. These states are believed to play key roles in the ground state properties and appear as low binding energy features. To explore such possibilities in the Fe-based systems, we study the core level spectra of a superconductor CaFe$_{1.9}$Co$_{0.1}$As$_2$ (CaCo122) in the CaFe$_2$As$_2$ (Ca122) family employing high-resolution hard x-ray photoemission spectroscopy. While As core levels show almost no change with doping and cooling, the Ca 2p peak of CaCo122 shows reduced surface contribution relative to Ca122 and a gradual shift of the peak position towards lower binding energies with cooling. In addition, we discover the emergence of a feature at the lower binding energy side of the well-screened Fe 2p signal in CaCo122. The intensity of this feature grows with cooling and indicates additional channels to screen the core holes. The evolution of this feature in the superconducting composition and its absence in the parent compound suggests relevance of the underlying interactions in the ground state properties of this class of materials. These results reveal another dimension in the studies of Fe-based superconductors and the importance of such states in the unconventional superconductivity in general