arXiv subjects

Asish K. Kundu

Publications and source records attributed to Asish K. Kundu.

At least 37 records · Page 2Linked to original sources

arXiv2024

Shallow core levels, or how to determine the doping and $T_c$ of Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ and Bi$_{2}$Sr$_2$CuO$_{6+δ}$ without cooling

Determining the doping level in high-temperature cuprate superconductors is crucial for understanding the origin of superconductivity in these materials and for unlocking their full potential. However, accurately determining the doping level remains a significant challenge due to a complex interplay of factors and limitations in various measurement techniques. In particular, in Bi$_{2}$Sr$_2$CuO$_{6+δ}$ and Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$, where the mobile carriers are introduced by non-stoichiometric oxygen $δ$, the determination has been extremely problematic. Here, we study the doping dependence of the electronic structure of these materials in angle-resolved photoemission and find that both the doping level, $p$, and the superconducting transition temeprature, $T_c$ can be precisely determined from the binding energy of the Bi $5d$ core-levels. The measurements can be performed at room temperature, enabling the determination of $p$ and $T_c$ without cooling the samples. This should be very helpful for further studies of these materials.

cond-mat.supr-con↗

arXiv2024

Giant Rashba-Splitting of One-Dimensional Metallic States in Bi Dimer Lines on InAs(100)

Bismuth produces different types of ordered superstructures on the InAs(100) surface, depending on the growth procedure and coverage. The (2x1) phase forms at completion of a Bi monolayer and consists of a uniformly oriented array of parallel lines of Bi dimers. Scanning tunneling and core level spectroscopies demonstrate its metallic character, in contrast with the semiconducting properties expected on the basis of the electron counting principle. The weak electronic coupling among neighboring lines gives rise to quasi one-dimensional Bi-derived bands with open contours at the Fermi level. Spin- and angle-resolved photoelectron spectroscopy reveals a giant Rashba splitting of these bands, in good agreement with ab-initio electronic structure calculations. The very high density of the dimer lines, the metallic and quasi one-dimensional band dispersion and the Rashba-like spin texture make the Bi/InAs(100)-(2x1) phase an intriguing system, where novel transport regimes can be studied.

cond-mat.mtrl-sci↗

arXiv2023

Coexistence of Dirac fermion and charge density wave in square-net-based semimetal LaAuSb2

We report a comprehensive study of magnetotransport properties, angle-resolved photoemission spectroscopy (ARPES), and density functional theory (DFT) calculations on self-flux grown LaAuSb$_2$ single crystals. Resistivity and Hall measurements reveal a charge density wave (CDW) transition at 77 K. MR and de Haas-Van Alphen (dHvA) measurements indicate that the transport properties of LaAuSb$_2$ are dominated by Dirac fermions that arise from Sb square nets. ARPES measurements and DFT calculations reveal an electronic structure with a common feature of the square-net-based topological semimetals, which is in good agreement with the magnetotransport properties. Our results indicate the coexistence of CDW and Dirac fermion in LaAuSb$_2$, both of which are linked to the bands arising from the Sb-square net, suggesting that the square net could serve as a structural motif to explore various electronic orders.

cond-mat.mtrl-sci↗

arXiv2023

Electronic structure, magnetic and transport properties of antiferromagnetic Weyl semimetal GdAlSi

We report the topological electronic structure, magnetic, and magnetotransport properties of a noncentrosymmetric compound GdAlSi. Magnetic susceptibility shows an antiferromagnetic transition at $T_\mathrm{N}$ = 32 K. In-plane isothermal magnetization exhibits an unusual hysteresis behavior at higher magnetic field, rather than near zero field. Moreover, the hysteresis behavior is asymmetric under positive and negative magnetic fields. First-principles calculations were performed on various magnetic configurations, revealing that the antiferromagnetic state is the ground state, and the spiral antiferromagnetic state is a close competing state. The calculations also reveal that GdAlSi hosts multiple Weyl points near the Fermi energy. The band structure measured by angle-resolved photoemission spectroscopy (ARPES) shows relatively good agreement with the theory, with the possibility of Weyl nodes slightly above the Fermi energy. Within the magnetic ordered state, we observe an exceptionally large anomalous Hall conductivity (AHC) of ~ 1310 $Ω^{-1}$cm$^{-1}$ at 2 K. Interestingly, the anomalous Hall effect persists up to room temperature with a significant value of AHC (~ 155 $Ω^{-1}$cm$^{-1}$). Our analysis indicates that the large AHC originates from the Berry curvature associated with the multiple pairs of Weyl points near Fermi energy.

cond-mat.str-el↗

arXiv2023

Spin Selective Evolution of Zhang-Rice State in Binary Transition Metal Oxide

The Zhang-Rice (ZR) state is a strongly hybridized bound state formed by the transition metal and oxygen atoms. The spin-fluctuations within the ZR state are known to play an important role in high-$T_\mathrm{c}$ superconductivity in cuprates. Here, we employ a combination of angle-resolved photoemission spectroscopy (ARPES), X-ray photoemission spectroscopy (XPS), and {\it ab initio} embedded dynamical mean-field theory (eDMFT) to investigate the influence of magnetic ordering on the spectral characteristics of the valence band and Mn 2$p$ core-level in MnO (001) ultrathin films. Our results demonstrate that a complex spin-selective evolution of Mn 3$d$$-$O 2$p$ hybridization develops due to the long-range antiferromagnetic (AFM) ordering. This hybridization significantly alters the spectral shape and weight of the ZR state. Specifically, in the AFM phase, we observed the sharpening of the ZR state and band folding with the periodicity of the AFM unit cell of MnO(001). We also demonstrated a strong connection between the spectral evolution of the ZR state and the non-local screening channels of the photoexcited core holes. Further, our detailed temperature-dependent study reveals the presence of short-range antiferromagnetic correlations that exist at much higher temperatures than $T_\mathrm{N}$. Such comprehensive studies showing the evolution of the ZR state across the magnetic transitions and its implication to the core-hole screening have never been reported in any 3$d$ binary transition metal oxides.

cond-mat.str-el↗

arXiv2023

Synthesis of a mesoscale ordered 2D-conjugated polymer with semiconducting properties

2D materials with high charge carrier mobility and tunable electronic band gaps have attracted intense research effort for their potential use as active components in nanoelectronics. 2D-conjugated polymers (2DCP) constitute a promising sub-class due to the fact that the electronic band structure can be manipulated by varying the molecular building blocks, while at the same time preserving the key features of 2D materials such as Dirac cones and high charge mobility. The major challenge for their use in technological applications is to fabricate mesoscale ordered 2DCP networks since current synthetic routes yield only small domains with a high density of defects. Here we demonstrate the synthesis of a mesoscale ordered 2DCP with semiconducting properties and Dirac cone structures via Ullmann coupling on Au(111). This material has been obtained by combining rigid azatriangulene precursors and a hot dosing approach which favours molecular diffusion and reduces the formation of voids in the network. These results open opportunities for the synthesis of 2DCP Dirac cone materials and their integration into devices.

cond-mat.mtrl-sci↗

arXiv2023

Interplay between local moment and itinerant magnetism in the layered metallic antiferromagnet TaFe$_{1.14}$Te$_3$

Two-dimensional (2D) antiferromagnets have garnered considerable interest for the next generation of functional spintronics. However, many available bulk materials from which 2D antiferromagnets are isolated are limited by their sensitivity to air, low ordering temperatures, and insulating transport properties. TaFe$_{1+y}$Te$_3$ offers unique opportunities to address these challenges with increased air stability, metallic transport properties, and robust antiferromagnetic order. Here, we synthesize TaFe$_{1+y}$Te$_3$ ($y$ = 0.14), identify its structural, magnetic, and electronic properties, and elucidate the relationships between them. Axial-dependent high-field magnetization measurements on TaFe$_{1.14}$Te$_3$ reveal saturation magnetic fields ranging between 27-30 T with a saturation magnetic moment of 2.05-2.12 $μ_B$. Magnetotransport measurements confirm TaFe$_{1.14}$Te$_3$ is metallic with strong coupling between magnetic order and electronic transport. Angle-resolved photoemission spectroscopy measurements across the magnetic transition uncover a complex interplay between itinerant electrons and local magnetic moments that drives the magnetic transition. We further demonstrate the ability to isolate few-layer sheets of TaFe$_{1.14}$Te$_3$ through mechanical exfoliation, establishing TaFe$_{1.14}$Te$_3$ as a potential platform for 2D spintronics based on metallic layered antiferromagnets.

cond-mat.mtrl-sci↗

arXiv2023

Electronic and magnetic properties of the topological semimetal SmMg$_2$Bi$_2$

Dirac semimetals show nontrivial physical properties and can host exotic quantum states like Weyl semimetals and topological insulators under suitable external conditions. Here, by combining angle-resolved photoemission spectroscopy measurements (ARPES) and first-principle calculations, we demonstrate that Zintl-phase compound SmMg$_2$Bi$_2$ belongs to the close proximity to a topological Dirac semimetallic state. ARPES results show a Dirac-like band crossing at the zone-center near the Fermi level ($E_\mathrm {F}$) which is further confirmed by first-principle calculations. Theoretical studies also reveal that SmMg$_2$Bi$_2$ belongs to a $Z_2$ topological class and hosts spin-polarized states around the $E_\mathrm {F}$. Zintl's theory predicts that the valence state of Sm in this material should be Sm$^{2+}$, however we detect many Sm-4$f$ multiplet states (flat-bands) whose energy positions suggest the presence of both Sm$^{2+}$ and Sm$^{3+}$. It is also evident that these flat-bands and other dispersive states are strongly hybridized when they cross each other. Due to the presence of Sm$^{3+}$ ions, the temperature dependence of magnetic susceptibility $χ(T)$ shows Curie-Weiss-like contribution in the low temperature region, in addition to the Van Vleck-like behaviour expected for the Sm$^{2+}$ ions. The present study will help in better understanding of the electronic structure, magnetism and transport properties of related materials.

cond-mat.str-el↗

arXiv2023

Anisotropic magnetism and electronic structure of trigonal EuAl$_2$Ge$_2$ single crystals

The magnetic and electronic properties of the layered Zintl-phase compound EuAl$_2$Ge$_2$ crystallizing in the trigonal CaAl$_2$Si$_2$-type structure are reported. Our neutron-diffraction measurements show that EuAl$_2$Ge$_2$ undergoes A-type antiferromagnetic (AFM) ordering below $T_{\rm N} = 27.5(5)$~K, with the Eu moments (Eu$^{2+}$, $S = 7/2$) aligned ferromagnetically in the $ab$ plane. The $H = 0$ magnetic structure consists of trigonal AFM domains associated with $ab$-plane magnetic anisotropy and a field-induced reorientation of the Eu spins in the domains is evident at $T = 2$~K below the critical field $H_{c1} = 2.5(1)$ kOe. Electrical resistivity and ARPES measurements show that EuAl$_2$Ge$_2$ is metallic both above and below $T_{\rm N}$. In the AFM phase, we directly observe folded bands in ARPES due to the doubling of the magnetic unit cell along the $c$ axis with an enhancement of quasiparticle weight due to the complex change in the coupling between the magnetic moments and itinerant electrons on cooling below $T_{\rm N}$. The observed electronic structure is well reproduced by first-principle calculations, which also predict the presence of nontrivial electronic states near the Fermi level in the AFM phase with $Z_2$ topological numbers 1;(000).

cond-mat.str-el↗

arXiv2022

Strongly-overdoped La$_{2-x}$Sr$_x$CuO$_4$: Evidence for Josephson-coupled grains of strongly-correlated superconductor

The interpretation of how superconductivity disappears in cuprates at large hole doping has been controversial. To address this issue, we present an experimental study of single-crystal and thin film samples of La$_{2-x}$Sr$_x$CuO$_4$ (LSCO) with $x\ge0.25$. In particular, measurements of bulk susceptibility on LSCO crystals with $x=0.25$ indicate an onset of diamagnetism at $T_{c1}=38.5$ K, with a sharp transition to a phase with full bulk shielding at $T_{c2}=18$ K, independent of field direction. Strikingly, the in-plane resistivity only goes to zero at $T_{c2}$. Inelastic neutron scattering on $x=0.25$ crystals confirms the presence of low-energy incommensurate magnetic excitations with reduced strength compared to lower doping levels. The ratio of the spin gap to $T_{c2}$ is anomalously large. Our results are consistent with a theoretical prediction for strongly overdoped cuprates by Spivak, Oreto, and Kivelson, in which superconductivity initially develops within disconnected self-organized grains characterized by a reduced hole concentration, with bulk superconductivity occurring only after superconductivity is induced by proximity effect in the surrounding medium of higher hole concentration. Beyond the superconducting-to-metal transition, local differential conductance measurements on an LSCO thin film suggest that regions with pairing correlations survive, but are too dilute to support superconducting order. Future experiments will be needed to test the degree to which these results apply to overdoped cuprates in general.

cond-mat.supr-con↗

arXiv2022

Topological electronic structure of YbMg$_2$Bi$_2$ and CaMg$_2$Bi$_2$

Zintl compounds have been extensively studied for their outstanding thermoelectric properties, but their electronic structure remains largely unexplored. Here, we present a detailed investigation of the electronic structure of the isostructural thermopower materials YbMg$_2$Bi$_2$ and CaMg$_2$Bi$_2$ using angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT). The ARPES results show a significantly smaller Fermi surface and Fermi velocity in CaMg$_2$Bi$_2$ than in YbMg$_2$Bi$_2$. Our ARPES results also reveal that in the case of YbMg$_2$Bi$_2$, Yb-4$f$ states reside well below the Fermi level and likely have a negligible impact on transport properties. To properly model the position of 4$f$-states, as well as the overall electronic structure, a Hubbard $U$ at the Yb sites and spin-orbit coupling (SOC) have to be included in the DFT calculations. Interestingly, the theoretical results reveal that both materials belong to a $Z_2$ topological class and host robust topological surface states around $E_\mathrm {F}$. Due to the intrinsic hole doping, the topological states reside above the Fermi level, inaccessible by ARPES. Our results also suggest that in addition to SOC, vacancies and the resulting hole doping play an important role in the transport properties of these materials.

cond-mat.mtrl-sci↗

arXiv2021

Quantum size effects, multiple Dirac cones and edge states in ultrathin Bi(110) films

The presence of inherently strong spin-orbit coupling in bismuth, its unique layer-dependent band topology and high carrier mobility make it an interesting system for both fundamental studies and applications. Theoretically, it has been suggested that strong quantum size effects should be present in the Bi(110) films, with the possibility of Dirac fermion states in the odd-bilayer (BL) films, originating from dangling $p_z$ orbitals and quantum-spin hall (QSH) states in the even-bilayer films. However, the experimental verification of these claims has been lacking. Here, we study the electronic structure of Bi(110) films grown on a high-$T_c$ superconductor, Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ (Bi2212) using angle-resolved photoemission spectroscopy (ARPES). We observe an oscillatory behavior of electronic structure with the film thickness and identify the Dirac-states in the odd-bilayer films, consistent with the theoretical predictions. In the even-bilayer films, we find another Dirac state that was predicted to play a crucial role in the QSH effect. In the low thickness limit, we observe several extremely one-dimensional states, probably originating from the edge-states of Bi(110) islands. Our results provide a much needed experimental insight into the electronic and structural properties of Bi(110) films.

cond-mat.mtrl-sci↗

arXiv2021

Role of surface termination in the metal-insulator transition of V$_2$O$_3$(0001) ultrathin films

Surface termination is known to play an important role in determining the physical properties of materials. It is crucial to know how surface termination affects the metal-insulator transition (MIT) of V$_2$O$_3$ films for both fundamental understanding and its applications. By changing growth parameters, we achieved a variety of surface terminations in V$_2$O$_3$ films that are characterized by low energy electron diffraction (LEED) and photoemission spectroscopy techniques. Depending upon the terminations, our results show MIT can be partially or fully suppressed near the surface region due to the different filling of the electrons at the surface and sub-surface layers and change of screening length compared to the bulk. Across MIT, a strong redistribution of spectral weight and its transfer from high-to-low binding energy regime is observed in a wide-energy-scale. Our results show total spectral weight in the low-energy regime is not conserved across MIT, indicating a breakdown of `sum rules of spectral weight', a signature of a strongly correlated system. Such change in spectral weight is possibly linked to the change in hybridization, lattice volume ({\it i.e.,} effective carrier density), and spin degree of freedom in the system that happens across MIT. We find that MIT in this system is strongly correlation-driven where the electron-electron interactions play a pivotal role. Moreover, our results provide a better insight in understanding the electronic structure of strongly correlated systems and highlight the importance of accounting surface effects during interpretation of the physical property data mainly using surface sensitive probes, such as surface resistivity.

cond-mat.str-el↗

arXiv2021

Hole-Like Fermi Surface in the Overdoped Non-Superconducting Bi$_{1.8}$Pb$_{0.4}$Sr$_2$CuO$_{6+δ}$

In high-temperature cuprate superconductors, the anti-ferromagnetic spin fluctuations are thought to have a very important role in naturally producing an attractive interaction between the electrons in the $d$-wave channel. The connection between superconductivity and spin fluctuations is expected to be especially consequential at the overdoped end point of the superconducting dome. In some materials, that point seems to coincide with a Lifshitz transition, where the Fermi surface changes from the hole-like centered at ($π, π$) to the electron-like, centered at the $Γ$ point causing a loss of large momentum anti-ferromagnetic fluctuations. Here, we study the doping dependence of the electronic structure of Bi$_{1.8}$Pb$_{0.4}$Sr$_2$CuO$_{6+δ}$ in angle-resolved photoemission and find that the superconductivity vanishes at lower doping than at which the Lifshitz transition occurs. This requires a more detailed re-examination of a spin-fluctuation scenario.

cond-mat.supr-con↗

arXiv2021

Homogeneous superconducting gap in DBCO synthesized by oxide molecular beam epitaxy

Much of what is known about high-temperature cuprate superconductors stems from studies based on two surface analytical tools, angle-resolved photoemission spectroscopy (ARPES) and spectroscopic imaging scanning tunneling microscopy (SI-STM). A question of general interest is whether and when the surface properties probed by ARPES and SI-STM are representative of the intrinsic properties of bulk materials. We find this question is prominent in thin films of a rarely studied cuprate DBCO. We synthesize DBCO films by oxide molecular beam epitaxy and study them by in situ ARPES and SI-STM. Both ARPES and SI-STM show that the surface DBCO layer is different from the bulk of the film. It is heavily underdoped, while the doping level in the bulk is close to optimal doping evidenced by bulk-sensitive mutual inductance measurements. ARPES shows the typical electronic structure of a heavily underdoped CuO2 plane and two sets of one-dimensional bands originating from the CuO chains with one of them gapped. SI-STM reveals two different energy scales in the local density of states, with one corresponding to the superconductivity and the other one to the pseudogap. While the pseudogap shows large variations over the length scale of a few nanometers, the superconducting gap is very homogeneous. This indicates that the pseudogap and superconductivity are of different origins.

cond-mat.supr-con↗

arXiv2020

Absence of a Dirac gap in ferromagnetic Cr$_x$(Bi$_{0.1}$Sb$_{0.9}$)$_{2-x}$Te$_3$

Magnetism breaks the time reversal symmetry expected to open a Dirac gap in 3D topological insulators that consequently leads to quantum anomalous Hall effect. The most common approach of inducing ferromagnetic state is by doping magnetic 3$d$ elements into bulk of 3D topological insulators. In Cr$_{0.15}$(Bi$_{0.1}$Sb$_{0.9}$)$_{1.85}$Te$_3$, the material where the quantum anomalous Hall effect was initially discovered at temperatures much lower than the ferromagnetic transition, $T_C$, the scanning tunneling microscopy studies have reported a large Dirac gap $\sim20-100$ meV. The discrepancy between the low temperature of quantum anomalous Hall effect ($\ll T_C$) and large spectroscopic Dirac gaps ($\gg T_C$) found in magnetic topological insulators remains puzzling. Here, we used angle-resolved photoemission spectroscopy to study the surface electronic structure of pristine and potassium doped surface of Cr$_{0.15}$(Bi$_{0.1}$Sb$_{0.9}$)$_{1.85}$Te$_3$. Upon potassium deposition, the $p$-type surface state of pristine sample was turned into an $n$-type, allowing spectroscopic observation of Dirac point. We find a gapless surface state, with no evidence of a large Dirac gap reported in tunneling studies.

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

Valence band electronic structure of the van der Waals ferromagnetic insulators: VI$_3$ and CrI$_3$

Ferromagnetic van der Waals (vdW) insulators are of great scientific interest for their promising applications in spintronics. It has been indicated that in the two materials within this class, CrI$_3$ and VI$_3$, the magnetic ground state, the band gap, and the Fermi level could be manipulated by varying the layer thickness, strain or doping. To understand how these factors impact the properties, a detailed understanding of the electronic structure would be required. However, the experimental studies of the electronic structure of these materials are still very sparse. Here, we present the detailed electronic structure of CrI$_3$ and VI$_3$ measured by angle-resolved photoemission spectroscopy (ARPES). Our results show a band-gap of the order of 1 eV, sharply contrasting some theoretical predictions such as Dirac half-metallicity and metallic phases, indicating that the intra-atomic interaction parameter (U) and spin-orbit coupling (SOC) were not properly accounted for in the calculations. We also find significant differences in the electronic properties of these two materials, in spite of similarities in their crystal structure. In CrI$_3$, the valence band maximum is dominated by the I 5{\it p}, whereas in VI$_3$ it is dominated by the V 3{\it d} derived states. Our results represent valuable input for further improvements in the theoretical modeling of these systems.

cond-mat.str-el↗