arXiv subjects

Ram Prakash Pandeya

Publications and source records attributed to Ram Prakash Pandeya.

At least 19 recordsLinked to original sources

arXiv2025

Overdoping YBa2Cu3O7 via a heterostructure with La0.67Sr0.33MnO3

YBa2Cu3Ox, the first superconductor discovered with Tc higher than 77 K, is among the most complex cuprates having both CuO chains and plains in the structure. YBa2Cu3O7 (YBCO) exhibits slightly overdoped behavior and further doping is difficult as all the lattice sites in the CuO chains are occupied. We have grown high quality single crystalline films of YBCO and bilayer La0.67Sr0.33MnO3 (LSMO)/YBCO exhibiting superconductivity in both the cases. Photoemission spectra reveal different surface and bulk electronic structures; the difference reduces in the bilayer. Evidence of charge transfer across the bilayer interface is observed in the valence band and core level spectra indicating an overdoped condition in YBCO. While superconductivity in the presence of magnetic order in the bilayer is puzzling, this pathway to reach overdoped regime in YBCO opens up a new landscape to probe the exotic physics of unconventional superconductivity.

cond-mat.supr-con↗

arXiv2024

Molecular order induced charge transfer in a C$_{60}$-topological insulator moiré heterostructure

We synthesize and spectroscopically investigate monolayer C$_{60}$ on the topological insulator (TI) Bi$_4$Te$_3$. This C$_{60}$/Bi$_4$Te$_3$ heterostructure is characterized by excellent translational order in a novel (4 x 4) C$_{60}$ superstructure on a (9 x 9) unit of Bi$_4$Te$_3$. We measure the full two-dimensional energy band structure of C$_{60}$/Bi$_4$Te$_3$ using angle-resolved photoemission spectroscopy (ARPES). We find that C$_{60}$ accepts electrons from the TI at room temperature but no charge transfer occurs at low temperatures. We unravel this peculiar behaviour by Raman spectroscopy of C$_{60}$/Bi$_4$Te$_3$ and density functional theory (DFT) calculations of the electronegativity of C$_{60}$. Both methods are sensitive to orientational order of C$_{60}$. At low temperatures, Raman spectroscopy shows a dramatic intensity increase of the C$_{60}$ Raman signal, evidencing a transition to a rotationally ordered state. DFT reveals that the orientational order of C$_{60}$ at low temperatures has a higher electron affinity than at high temperatures. These results neatly explain the temperature-dependent charge transfer observed in ARPES. Our conclusions are supported by the appearance of a strong photoluminescence from C$_{60}$/Bi$_4$Te$_3$ at low temperatures.

cond-mat.mtrl-sci↗

arXiv2024

Evidence of electron correlation and unusual spectral evolution in an exotic superconductor, PdTe

We study the electronic structure of an exotic superconductor, PdTe employing depth-resolved high resolution photoemission spectroscopy and density functional theory. The valence band spectra exhibit large density of states at the Fermi level with flat intensity in a wide energy range indicating highly metallic ground state. The Pd 4d-Te 5p hybridization is found to be strong leading to a highly covalent character of the itinerant states. Core level spectra exhibit several features including the signature of plasmon excitations. Although the radial extension of the 4d orbitals is larger than 3d ones, the Pd core level spectra exhibit distinct satellites indicating importance of electron correlation in the electronic structure which may be a reason for unconventional superconductivity observed in this system. The depth-resolved data reveal surface peaks at higher binding energies in both, Te and Pd core level spectra. Interestingly, core level shift in Te-case is significantly large compared to Pd although Te is relatively more electronegative. Detailed analysis rules out applicability of the charge transfer and/or band-narrowing models to capture this scenario. This unusual scenario is attributed to the reconstruction and/or vacancies at the surface. These results reveal the importance of electron correlation and surface topology for the physics of this material exhibiting Dirac fermions and complex superconductivity.

cond-mat.supr-con↗

arXiv2023

Evidence of charge transfer in a bilayer film, LaSrMnO3/YBa2Cu3O7

We study the growth and electronic properties of a high temperature superconductor, YBa$_2$Cu$_3$O$_7$ (YBCO) in proximity of a magnetic material, La$_{0.67}$Sr$_{0.33}$MnO$_3$ (LSMO). High quality single crystalline films of YBCO and LSMO/YBCO were grown epitaxially on SrTiO$_3$ (001) surface. Magnetization data of the LSMO/YBCO bilayer exhibit ferromagnetic ordering with Curie temperature smaller than that of pure LSMO. Measurements at different field directions reveal emergence of an anisotropy at low temperatures with in-plane easy axis; the observed anisotropy is stronger in the superconducting region. Magnetization data of YBCO exhibit onset of diamagnetism at 86 K for the out-of-plane magnetic measurements while the in-plane measurements show onset at a slightly higher temperature of 89 K with much smaller moment. Interestingly, the onset of diamagnetism in LSMO/YBCO film remains at 86 K despite the presence of ferromagnetic LSMO layer underneath. The analysis of Ba 4$d$ and Y 3$d$ core level spectra suggest that the surface and bulk electronic structure in these systems are different; the difference is reduced significantly in the LSMO/YBCO sample suggesting an enhancement of electron density near the surface arising from the charge transfer across the interface, which is consistent with the magnetization data.

cond-mat.supr-con↗

arXiv2023

Complexity in the hybridization physics revealed by depth-resolved photoemission spectroscopy of single crystalline novel Kondo lattice systems, CeCuX$_2$ (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.

cond-mat.str-el↗

arXiv2023

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.

cond-mat.str-el↗

arXiv2022

Behavior of gapped and ungapped Dirac cones in an antiferromagnetic topological metal, SmBi

We studied the behavior of nontrivial Dirac fermion states in an antiferromagnetic metal SmBi using angle-resolved photoemission spectroscopy (ARPES). The experimental results exhibit multiple Fermi pockets around $\overlineΓ$ and $\overline{M}$ points along with a band inversion in the spectrum along the $\overlineΓ$-$\overline{M}$ line consistent with the density functional theory results. In addition, ARPES data reveal Dirac cones at $\overlineΓ$ and $\overline{M}$ points within the energy gap of the bulk bands. The Dirac cone at $\overline{M}$ exhibit a distinct Dirac point and is intense in the high photon energy data while the Dirac cone at $\overlineΓ$ is intense at low photon energies. Employing ultra-high-resolution ARPES, we discover destruction of a Fermi surface constituted by the surface states across the Neél temperature of 9 K. Interestingly, the Dirac cone at $\overlineΓ$ is found to be gapped at 15 K and the behavior remains similar across the magnetic transition. These results reveal complex momentum dependent gap formation and fermi surface destruction across magnetic transition in an exotic correlated topological material; the interplay between magnetism and topology in this system calls for ideas beyond existing theoretical models.

cond-mat.str-el↗

arXiv2022

Giant spectral renormalization and complex hybridization physics in a Kondo lattice system, CeCuSb2

We investigate the electronic structure of a Kondo lattice system, CeCuSb2 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 non-equivalent 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.

cond-mat.str-el↗

arXiv2021

Anomalies in the electronic structure of a 5$d$ transition metal oxide, IrO$_2$

Ir-based materials have drawn much attention due to the observation of insulating phase believed to be driven by spin-orbit coupling while Ir 5$d$ states are expected to be weakly correlated due to their large orbital extensions. IrO$_2$, a simple binary material, shows metallic ground state which seems to deviate from the behavior of most other Ir-based materials and varied predictions in these material class. We studied the electronic structure of IrO$_2$ at different temperatures employing high resolution photoemission spectroscopy with photon energies spanning from ultraviolet to hard $x$-ray range. Experimental spectra exhibit a signature of enhancement of Ir-O covalency in the bulk compared to the surface electronic structure. The branching ratio of the spin-orbit split Ir core level peaks is found to be larger than its atomic values and it enhances further in the bulk electronic structure. Such deviation from the atomic description of the core level spectroscopy manifests the enhancement of the orbital moment due to the solid state effects. The valence band spectra could be captured well within the density functional theory. The photon energy dependence of the features in the valence band spectra and their comparison with the calculated results show dominant Ir 5$d$ character of the features near the Fermi level; O 2$p$ peaks appear at higher binding energies. Interestingly, the O 2$p$ contributions of the feature at the Fermi level is significant and it enhances at low temperatures. This reveals an orbital selective enhancement of the covalency with cooling which is an evidence against purely spin-orbit coupling based scenario proposed for these systems.

cond-mat.str-el↗

arXiv2021

Emergence of well screened states in a superconducting material of the CaFe$_2$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, Ca 2$p$ peak of CaCo122 show reduced surface contribution relative to Ca122 and a gradual shift of the peak position towards lower binding energies with cooling. In addition, we discover emergence of a feature at lower binding energy side of the well screened Fe 2$p$ signal in CaCo122. The intensity of this feature grows with cooling and indicate additional channels to screen the core holes. The evolution of this feature in the superconducting composition and it's absence in the parent compound suggests relevance of the underlying interactions in the ground state properties of this class of materials. These results reveal a new dimension in the studies of Fe-based superconductors and the importance of such states in the unconventional superconductivity in general.

cond-mat.supr-con↗

arXiv2021

Anomalies in the temperature evolution of the Dirac states in a topological crystalline insulator SnTe

Discovery of topologically protected surface states, believed to be immune to weak disorder and thermal effects, opened up a new avenue to reveal exotic fundamental science and advanced technology. While time-reversal symmetry plays the key role in most such materials, the bulk crystalline symmetries such as mirror symmetry preserve the topological properties of topological crystalline insulators (TCIs). It is apparent that any structural change may alter the topological properties of TCIs. To investigate this relatively unexplored landscape, we study the temperature evolution of the Dirac fermion states in an archetypical mirror-symmetry protected TCI, SnTe employing high-resolution angle-resolved photoemission spectroscopy and density functional theory studies. Experimental results reveal a perplexing scenario; the bulk bands observed at 22 K move nearer to the Fermi level at 60 K and again shift back to higher binding energies at 120 K. The slope of the surface Dirac bands at 22 K becomes smaller at 60 K and changes back to a larger value at 120 K. Our results from the first-principles calculations suggest that these anomalies can be attributed to the evolution of the hybridization physics with complex structural changes induced by temperature. In addition, we discover drastically reduced intensity of the Dirac states at the Fermi level at high temperatures may be due to complex evolution of anharmonicity, strain, etc. These results address robustness of the topologically protected surface states due to thermal effects and emphasize importance of covalency and anharmonicity in the topological properties of such emerging quantum materials.

cond-mat.mtrl-sci↗

arXiv2020

Exceptional Dirac states in a non-centrosymmetric superconductor, BiPd

Quantum materials having Dirac fermions in conjunction with superconductivity is believed to be the candidate materials to realize exotic physics as well as advanced technology. Angle resolved photoemission spectroscopy (ARPES), a direct probe of the electronic structure, has been extensively used to study these materials. However, experiments often exhibit conflicting results on dimensionality and momentum of the Dirac Fermions (e.g. Dirac states in BiPd, a novel non-centrosymmetric superconductor), which is crucial for the determination of the symmetry, time-reversal invariant momenta and other emerging properties. Employing high-resolution ARPES at varied conditions, we demonstrated a methodology to identify the location of the Dirac node accurately and discover that the deviation from two-dimensionality of the Dirac states in BiPd proposed earlier is not a material property. These results helped to reveal the topology of the anisotropy of the Dirac states accurately. We have constructed a model Hamiltonian considering higher-order spin-orbit terms and demonstrate that this model provides an excellent description of the observed anisotropy. Intriguing features of the Dirac states in a non-centrosymmetric superconductor revealed in this study expected to have significant implication in the properties of topological superconductors.

cond-mat.supr-con↗

arXiv2020

Structural anomaly in superconductivity of CaFe2As2 class of materials

Quantum transitions in Fe-based systems are believed to involve spin, charge and nematic fluctuations. Complex structural phase diagram in these materials often emphasizes importance of covalency in their exotic properties, which is directly linked to the local structural network and barely understood. In order to address this outstanding issue, we investigate the evolution of 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 Fe K- and As K-absorption edge of CaFe2As2 and its superconducting composition, CaFe1.9Co0.1As2 (Tc = 12 K) exhibit evidence of enhancement of Fe contribution with Co-substitution near the Fermi level. As-Fe and Fe-Fe bondlengths derived from the experimental data exhibit interesting changes with temperature across the magneto-structural transition. Curiously, the evolution in Co-doped composition is similar to its parent compound despite absence of magneto-structural transition. In addition, we discover anomalous change of Ca-X (X = Fe, As) bondlengths with temperature in the vicinity of magneto-structural transition and disorder appears to be less important presumably due to screening by the charge reservoir layer. These results reveal evidence of doping induced evolution to the proximity to critical behavior presumably leading to superconductivity in the system.

cond-mat.supr-con↗

arXiv2020

Preparation, characterization and X-ray photoemission spectroscopy study of a correlated semimetal, SmBi

We report high quality single crystalline growth of SmBi using flux method. The compound crystallizes in the simple rock salt structure with space group Fm3m. The cubic structure of the single crystal was confirmed by Laue diffraction pattern. The magnetic susceptibility measurements reveal sharp antiferromagnetic order with Neel temperature of 9 K. The core level photoemission spectroscopy study of Sm 3d has been performed using monochromatic Al Kalpha source. We observe multiple features in the experimental spectra due to fonal state effect - a signature of hybridization between Sm 4f - Bi 6p states. Intense satellite features are also observed presumably due to mixed valency arising from Kondo coupling. No signature of surface-bulk difference is observed in the Sm 3d core level spectra.

cond-mat.str-el↗

arXiv2020

Unusual role of ligand states in the electronic properties of a parent Fe-based superconductor, CaFe2As2

We investigate the role of ligand states in the electronic properties of CaFe2As2 using high-resolution hard x-ray photoemission spectroscopy (HAXPES) at different sample temperatures. Experimental results indicate that the binding energy of Ca is close to that for 2+ charge state of Ca atoms and the other constituent elements, Fe and As possess electronic configuration close to that in elemental systems. No difference is observed in the As 3p core level spectra with the change of emission angle and/or the change in sample temperature. This is surprising as the Ca atoms at the cleaved sample surface reorganizes itself to form linear structures which is expected to influence Ca-As hybridization leading to significant difference in surface and bulk electronic structures. Moreover, CaFe2As2 undergoes structural and magnetic phase transition at 170 K, and strong Fe-As hybridization provides pathways for electron dynamics. Clearly, further studies are required to resolve these puzzling observations.

cond-mat.supr-con↗

arXiv2020

Anomalous spectral evolution with bulk sensitivity in BiPd

We investigate the electronic structure of a noncentrosymmetric superconductor, BiPd using photoemission spectroscopy with multiple photon energies ranging from ultraviolet to hard x-ray. Experimental data exhibit interesting difference in the surface and bulk electronic structures of this system. While the surface Bi core level peaks appear at lower binding energies, the surface valence band features are found at the higher binding energy side of the bulk valence band; valence band is primarily constituted by the Pd 4d states. These changes in the electronic structure cannot be explained by the change in ionicity of the constituent elements via charge transfer. Analysis of the experimental data indicates that the Bi-Pd hybridization physics plays the key role in deriving the anomalous spectral evolution and the electronic properties of this system.

cond-mat.mtrl-sci↗

arXiv2020

Preparation, Characterization and electronic structure of Ti-doped Bi$_2$Se$_3$

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.

cond-mat.mtrl-sci↗

arXiv2020

On-demand local modification of high-$T_\text{c}$ superconductivity in few unit-cell thick Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$

High-temperature superconductors (HTS) are important for potential applications and for understanding the origin of strong correlations. Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ (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, will be of immense interest for superconducting electronics. Here we report transport studies on few unit-cell thick BSCCO and modify its superconductivity locally by depositing metal on the surface. Deposition of chromium (Cr) on the surface over a selected area of BSCCO results in insulating behavior of the patterned region. Cr locally depletes oxygen in CuO$_2$ planes and disrupts the superconductivity in the layers below. Our technique of modifying superconductivity is suitable for making sub-micron superconducting wires and more complex superconducting electronic devices.

cond-mat.supr-con↗