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Indra Dasgupta

Publications and source records attributed to Indra Dasgupta.

34 records · Page 2Linked to original sources

Spin-orbit effects in pentavalent Iridates: Models and materials

Spin-orbit effects in heavy 5$d$ transition metal oxides, in particular, iridates, have received enormous current interest due to the prediction as well as the realization of a plethora of exotic and unconventional magnetic properties. While a bulk of these works are based on tetravalent iridates ($d^5$), where the counter-intuitive insulating state of the rather extended 5$d$ orbitals are explained by invoking strong spin-orbit coupling, the recent quest in iridate research has shifted to the other valencies of Ir, of which pentavalent iridates constitute a notable representative. In contrast to the tetravalent iridates, spin-orbit entangled electrons in $d^4$ systems are expected to be confined to the $J = 0$ singlet state without any resultant moment or magnetic response. However, it has been recently predicted that, magnetism in $d^4$ systems may occur via magnetic condensation of excitations across spin-orbit-coupled states. In reality, the magnetism in Ir$^{5+}$ systems are often quite debatable both from theoretical as well as experimental point of view. Here we provide a comprehensive overview of the spin-orbit coupled $d^4$ model systems and its implications in the studied pentavalent iridates. In particular, we review here the current experimental and theoretical understanding of the double perovskite ($A_2B$YIrO$_6$, $A =$ Sr, Ba, $B =$Y, Sc, Gd), 6H-perovskite (Ba$_3M$Ir$_2$O$_9$, $M =$ Zn, Mg, Sr, Ca), post-perovskite (NaIrO$_3$), and Hexagonal (Sr$_3$MIrO$_6$) iridates, along with a number of open questions that require future investigation.

cond-mat.str-el↗

Superconductivity in Infinite-layer Nickelates : Role of Non-zero f-ness

Employing first-principles density functional theory calculations and Wannierization of the low energy band structure, we analyze the electronic structure of undoped, infinite-layer nickelate compounds, NdNiO$_2$, PrNiO$_2$ and LaNiO$_2$. Our study reveals important role of non-zero $f$-ness of Nd and Pr atoms, as opposed to $f^{0}$ occupancy of La. The non-zero $f$-ness becomes effective in lowering the energy of the rare-earth 5$d$ hybridized axial orbital, thereby enhancing the electron pockets and influencing the Fermi surface topology. The Fermi surface topology of NdNiO$_2$ and PrNiO$_2$ is strikingly similar, while differences are observed for LaNiO$_2$. This difference shows up in computed doping dependent superconducting properties of the three compounds within a weak coupling theory. We find two gap superconductivity for NdNiO$_2$ and PrNiO$_2$, and possibility of a single gap superconductivity for LaNiO$_2$ with the strength of superconductivity suppressed by almost a factor of two, compared to Nd or Pr compound.

cond-mat.supr-con↗

Electronic structure and transport properties of coupled CdS/ZnSe quantum dots

Electronic structure and transport characteristics of coupled CdS and ZnSe quantum dots are studied using density functional theory and non equilibrium Greens function method respectively. Our investigations show that in these novel coupled dots, the frontier occupied and unoccupied molecular orbitals are spatially located in two different parts of the coupled dot, thereby indicating the possibility of asymmetry in electronic transport. We have calculated electronic transport through the coupled quantum dot by varying the coupling strength between the individual quantum dots in the limits of weak and strong coupling. Calculations reveal asymmetric current vs voltage curves in both the limits indicating the rectifying properties of the coupled quantum dots. Additionally we discuss the possibility to tune the switching behavior of the coupled dots by different gate geometries.

cond-mat.mes-hall↗

Understanding the Curious Magnetic State of Sr$_{3}$OsO$_{6}$

Motivated by the recent report on high T$_c$ ferromagnetic insulating state of single transition metal containing double perovskite compound, Sr$_3$OsO$_6$ (Wakabayashi et. al., Nature Commun {\bf 10} 535, 2019), we study this curious behavior by employing first-principles calculations in conjunction with exact diagonalization of full $t_{2g}$ multiplet problem of two Os sites. Our analysis highlights the fact that stabilization of Sr$_3$OsO$_6$ in the cubic phase in epitaxially grown thin film is the key to both ferromagnetic correlation and high temperature scale associated to it. This also provides a natural explanation for the sister compound, Ca$_3$OsO$_6$ to exhibit low T$_N$ antiferromagnetism in its monoclinic structure. Further the insulating property is found to be driven by opening of Mott gap in the half filled spin-orbit coupled $j=3/2$ manifold of $d^{2}$ Os. We point out that Sr$_2$CaOsO$_6$ which naturally forms in the cubic phase would be worthwhile to explore as a future candidate to exhibit high T$_c$ ferromagnetic insulating state in bulk form.

cond-mat.str-el↗

Orbital Selective Superconductivity in a Two-band Model of Infinite-Layer Nickelates

In the present study, we explore superconductivity in NdNiO$_2$ and LaNiO$_2$ employing a first-principles derived low-energy model Hamiltonian, consisting of two orbitals: Ni $x^{2}$-$y^{2}$, and an {\it axial} orbital. The {\it axial} orbital is constructed out of Nd/La $d$, Ni 3$z^{2}$-$r^{2}$ and Ni $s$ characters. Calculation of the superconducting pairing symmetry and pairing eigenvalue of the spin-fluctuation mediated pairing interaction underlines the crucial role of inter-orbital Hubbard interaction in superconductivity, which turns out to be orbital-selective. The axial orbital brings in materials dependence in the problem, making NdNiO$_2$ different from LaNiO$_2$, thereby controlling the inter-orbital Hubbard interaction assisted superconductivity.

cond-mat.supr-con↗

Hybridization-switching induced Mott transition in ABO$_3$ perovskites

We propose the concept of "hybridization-switching induced Mott transition" which is relevant to a broad class of ABO$_3$ perovskite materials including BiNiO$_3$ and PbCrO$_3$ which feature extended $6s$ orbitals on the A-site cation (Bi or Pb), and A-O covalency induced ligand holes. Using {\it ab initio} electronic structure and slave rotor theory calculations, we show that such systems exhibit a breathing phonon driven A-site to oxygen hybridization-wave instability which conspires with strong correlations on the B-site transition metal ion (Ni or Cr) to induce a Mott insulator. These Mott insulators with active A-site orbitals are shown to undergo a pressure induced insulator to metal transition accompanied by a colossal volume collapse due to ligand hybridization switching.

cond-mat.str-el↗

Development of half metallicity within mixed magnetic phase of Cu$_{1-x}$Co$_x$MnSb alloy

Cubic Half-Heusler Cu$_{1-x}$Co$_x$MnSb (0 $\leq$ $x$ $\leq$ 0.1) compounds have been investigated both experimentally and theoretically for their magnetic, transport and electronic properties in search of possible half metallic antiferromagnetism. The systems (Cu,Co)MnSb are of particular interest as the end member alloys CuMnSb and CoMnSb are semi metallic (SM) antiferromagnetic (AFM) and half metallic (HM) ferromagnetic (FM), respectively. Clearly, Co-doping at the Cu-site of CuMnSb introduces changes in the carrier concentration at the Fermi level that may lead to half-metallic ground state but there remains a persistent controversy whether the AFM to FM transition occurs simultaneously. Our experimental results reveal that the AFM to FM magnetic transition occurs through a percolation mechanism where Co-substitution gradually suppresses the AFM phase and forces FM polarization around every dopant cobalt. As a result a mixed magnetic phase is realized within this composition range while a nearly HM band structure is developed already at the 10% Co-doping. Absence of T$^2$ dependence in the resistivity variation at low T-region serves as an indirect proof of opening up an energy gap at the Fermi surface in one of the spin channels. This is further corroborated by the ab-initio electronic structure calculations that suggests a nearly ferromagnetic half-metallic ground state is stabilized by Sb-p holes produced upon Co doping.

cond-mat.str-el↗

Electronic, magnetic and ferroelectric properties of rhombohedral AgFeO2: an ab initio study

Using first principle calculations under the framework of density functional theory we have investigated the electronic structure, magnetism and ferroelectric polarization in the triangular lattice antiferromagnet AgFeO2, and its comparison to the isostructural system CuFeO2. Our calculations reveal that spin orbit interaction plays an important role in determining the magnetic property of AgFeO2 and is possibly responsible for its different magnetic ground state in comparison to CuFeO2. Calculations of ferroelectric polarization of AgFeO2 suggest that the spontaneous polarization arises from noncollinear spin arrangement via spin-orbit coupling. Our calculations also indicate that in addition to electronic contribution, the lattice mediated contribution to the polarization are also important for AgFeO2.

cond-mat.mtrl-sci↗

Spin-orbital liquid state assisted by singlet-triplet excitation in $J~=~0$ ground state of Ba$_3$ZnIr$_2$O$_9$

Strong spin-orbit coupling (SOC) effects of heavy $d$-orbital elements have long been neglected in describing the ground states of their compounds thereby overlooking a variety of fascinating and yet unexplored magnetic and electronic states, until recently. The spin-orbit entangled electrons in such compounds can get stabilized into unusual spin-orbit multiplet $J$-states which warrants severe investigations. Here we show using detailed magnetic and thermodynamic studies and theoretical calculations the ground state of Ba$_3$ZnIr$_2$O$_9$, a 6$H$ hexagonal perovskite is a close realisation of the elusive $J$~=~0 state. However, we find that local Ir moments are spontaneously generated due to the comparable energy scales of the singlet-triplet splitting driven by SOC and the superexchange interaction mediated by strong intra-dimer hopping. While the Ir ions within the structural Ir$_2$O$_9$ dimer prefers to form a spin-orbit singlet state (SOS) with no resultant moment, substantial interdimer exchange interactions from a frustrated lattice ensure quantum fluctuations till the lowest measured temperatures and stabilize a spin-orbital liquid phase.

cond-mat.str-el↗

Strain induced band alignment in wurtzite-zincblende InAs heterostructured nanowires

We study band alignment in wurtzite-zincblende polytype InAs heterostructured nanowires using temperature dependent resonance Raman measurements. Nanowires having two different wurtzite fractions are investigated. Using visible excitation wavelengths in resonance Raman measurements, we probe the electronic band alignment of these semiconductor nanowires near a high symmetry point of the Brillouin zone (E$_{1}$ gap). The strain in the crystal structure, as revealed from the shift of the phonon mode, explains the observed band alignment at the wurtzite-zincblende interface. Our experimental results are further supported by electronic structure calculations for such periodic heterostructured interface.

cond-mat.mtrl-sci↗

Role of Te in the low dimensional multiferroic material FeTe2O5Br

Using first principles density functional calculations, we study the electronic structure of the low-dimensional multiferroic compound FeTe2O5Br to investigate the origin of the magnetoelectric (ME) effect and the role of Te ions in this system. We find that without magnetism even in the presence of Te-5s lone pairs, the system remains centrosymmetric due to the antipolar orientation of the lone pairs. Our study shows that the exchange striction within the Fe tetramers as well as between them is responsible for the ME effect in FeTe2O5Br. We also find that the Te^4+ ions play an important role in the inter-tetramer exchange striction as well as contribute to the electric polarization in FeTe2O5Br, once the polarization is triggered by the magnetic ordering.

cond-mat.mtrl-sci↗

Magnetic properties of Mn-doped Ge46 and Ba8Ge46 clathrates

We present a detailed study of the magnetic properties of unique cluster assembled solids namely Mn doped Ge46 and Ba8Ge46 clathrates using density functional theory. We find that ferromagnetic (FM) ground states may be realized in both the compounds when doped with Mn. In Mn2Ge44, ferromagnetism is driven by hybridization induced negative exchange splitting, a generic mechanism operating in many diluted magnetic semiconductors. However, for Mn-doped Ba8Ge46 clathrates incorporation of conduction electrons via Ba encapsulation results in RKKY-like magnetic interactions between the Mn ions. We show that our results are consistent with the major experimental observations for this system.

cond-mat.mtrl-sci↗

LaSrVMoO$_6$: A case study for $A$-site covalency-driven local cationic order in double perovskites

An unusual atomic scale chemical fluctuation in LaSrVMoO$_6$, in terms of narrow patches of La,V and Sr,Mo-rich phases, has been probed in detail to understand the origin of such a chemical state. Exhaustive tuning of the equilibrium synthesis parameters showed that the extent of phase separation can never be melted down below an unit cell dimension making it impossible to achieve the conventional $B$-site ordered structure, which establishes that the observed `inhomogeneous' patch-like structure with minimum dimension of few angstroms is a reality in LaSrVMoO$_6$. Therefore, another type of local chemical order, hitherto unknown in double perovskites, gets introduced here. X-ray diffraction, electron microscopy elemental mapping, magnetic, and various spectroscopic studies have been carried out on samples, synthesized under different conditions. These experimental results in conjunction with {\it ab-initio} electronic structure calculation revealed that it is the energy stability, gained by typical La-O covalency as in LaVO$_3$, that leads to the preferential La,V and Sr,Mo ionic proximity, and the consequent patchy structure.

cond-mat.mtrl-sci↗

Atomic scale chemical fluctuation in LaSrVMoO6: A proposed halfmetallic antiferromagnet

Half metallic antiferromagnets (HMAFM) have been proposed theoretically long ago but have not been realized experimentally yet. Recently, a double perovskite compound, LaSrVMoO6, has been claimed to be an almost real HMAFM system. Here, we report detailed experimental and theoretical studies on this compound. Our results reveal that the compound is neither a half metal nor an ordered antiferromagnet. Most importantly, an unusual chemical fluctuation is observed locally, which finally accounts for all the electronic and magnetic properties of this compound.

cond-mat.mtrl-sci↗

Electronic structure and magnetism of transition metal doped Zn12O12 clusters: Role of defects

We present a comprehensive study of the energetics and magnetic properties of ZnO clusters doped with 3d transition metals (TM) using ab initio density functional calculations in the framework of generalized gradient approximation + Hubbard U (GGA+U) method. Our results within GGA+U for all 3d dopants except Ti indicate that antiferromagnetic interaction dominates in a neutral, defect-free cluster. Formation energies are calculated to identify the stable defects in the ZnO cluster. We have analyzed in details the role of these defects to stabilize ferromagnetism when the cluster is doped with Mn, Fe, and Co. Our calculations reveal that in the presence of charged defects the transition metal atoms residing at the surface of the cluster may have an unusual oxidation state, that plays an important role to render the cluster ferromagnetic. Defect induced magnetism in ZnO clusters without any TM dopants is also analyzed. These results on ZnO clusters may have significant contributions in the nanoengineering of defects to achieve desired ferromagnetic properties for spintronic applications.

cond-mat.mtrl-sci↗

The making of ferromagnetic Fe doped ZnO nano-clusters

In this letter, the authors present a study of the energetics and magnetic interactions in Fe doped ZnO clusters by ab-initio density functional calculations. The results indicate that defects under suitable conditions can induce ferromagnetic interactions between the dopant Fe atoms whereas antiferromagnetic coupling dominates in a neutral defect-free cluster. The calculations also reveal an unusual ionic state of the dopant Fe atom residing at the surface of the cluster, a feature that is important to render the cluster ferromagnetic.

cond-mat.mtrl-sci↗