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R. Bindu

Publications and source records attributed to R. Bindu.

At least 19 recordsLinked to original sources

Coupling of magnetism and transport properties to the lattice degrees of freedom in NdBaCo$_2$O$_{5+{\delta}}$ ($\delta \sim 0.65$)

We have studied the origin of zero volume expansion below the Curie temperature (Tc), variable range hopping (VRH) behaviour using structural, magnetic, transport and thermal studies on the oxygen deficient double perovskite NdBaCo$_2$O$_{5+{\delta}}$ ($\delta \sim 0.65$). The valence state of Co ions and the possible properties exhibited by such compound were studied using electronic structure calculations for $\delta = 0.75$. Careful investigation of structure shows that the compound stabilizes in tetragonal structure (P4/mmm) having $2a_p \times 2a_p \times 2a_p$ (222) superstructure, where $a_p$ is the cubic perovskite lattice parameter. The compound exhibits a minimum in resistivity, ferromagnetic and ferrimagnetic transitions around 375 K, 120 K ($T_c$) and 60 K, respectively with signature of Griffiths phase above $T_c$. Our detailed structural analysis suggests signature of the onset of the above magnetic transitions at temperatures well above its stabilisation at long range level thereby leading to VRH behaviour. The observed zero thermal expansion in volume below Tc appears to be due to competing magnetic interactions within and between the magnetic sublattices. Our electronic structure calculations show (a) the importance of electron-electron correlation in Nd $4f$ and Co $3d$ states (b) Co ions stabilize in intermediate spin (IS) state, having oxidation state less than +3 (c) half metallicity. Our results show the possibility of coupling between magnetism and ferroelectricity. We believe that our results especially on the valence state of the Co ion, zero thermal expansion in volume, short range magnetic orderings and the connection between different degrees of freedom will be helpful in clearing the ambiguities existing in literature on the nature of magnetism and thereby aiding in designing new functionalities.

cond-mat.str-el

Evidence of Lattice Strain as a Precursor to Superconductivity in BaPb$_{0.75}$Bi$_{0.25}$O$_3$

In this work, we have investigated the precursor effects to superconductivity in BaPb$_{0.75}$Bi$_{0.25}$O$_3$ using temperature dependent resistivity, x-ray diffraction technique and photoemission spectroscopy. The present compound exhibits superconductivity around 11 K ($T_C$). The synthesis procedure adopted is much simpler as compared to the procedure available in the literature. In the temperature range (10 K-25 K) i.e. above $T_C$, our results show an increase in both the orthorhombic and tetragonal strain. The well screened features observed in Bi and Pb 4$f_{7/2}$ core levels are indicative of the metallic nature of the sample. The compound exhibits finite intensity at the Fermi level at 300 K and this intensity decreases with decrease in temperature and develops into a pseudogap; the energy dependence of the spectral density of states suggests disordered metallic state. Furthermore, our band structure calculations reveal that the structural transition upon Pb doping results in the closing of the band gap at the Fermi level.

cond-mat.supr-con

Tuning the structural, electronic and magneto-transport properties of spin-orbit Mott insulator Sr2IrO4

We investigate the tunability of the structural, electronic and magneto transport properties of polycrystalline Sr2IrO4 sample. The extent of bifurcation of the magnetisation curves during the field cooled and zero field cooled cycles establishes that the magnetic anisotropy in the as-prepared sample is more as compared to the vacuum annealed one. Based on the behaviours of the structural parameters and the magnetic studies, our results show that the canted AFM structure is stabilised in a larger temperature range in the case of the annealed sample as compared to the as prepared one. At low temperatures, for both the samples, a phase, possibly of glassy nature competes with the canted AFM phase. The temperature extent to which both these phases co-exist for the as-prepared and the annealed one is around 115K an 70K, respectively. The transport studies reveal that for both the samples, in the high temperature region of study, the conduction mechanism is governed by the Arrhenius model. In the intermediate temperature range, variable range hopping(VRH) and Arrhenius models govern the transport in the as-prepared and the annealed one, respectively. At low temperatures, the conduction mechanism occurs through Efros-Shklovskii-VRH and VRH mechanisms for the as-prepared and the annealed samples, respectively. The magneto resistance measurements indicate higher negative magneto resistance in the annealed sample at all temperatures. The field dependence of magneto resistance at 10K suggests a co-existing glassy magnetic phase along with the canted antiferromagnetic structure in the as prepared sample and a suppression of this glassy magnetic phase in the annealed sample. The combined analyses of all the results highlight the role of disorder for the magnetic and trasnport properties of this compound.

cond-mat.str-el

Tetramer Orbital-Ordering induced Lattice-Chirality in Ferrimagnetic, Polar MnTi2O4

Using density-functional theory calculations and experimental investigations on structural, magnetic and dielectric properties, we have elucidated a unique tetragonal ground state for MnTi2O4, a Ti^{3+} (3d^1)-ion containing spinel-oxide. With lowering of temperature around 164 K, cubic MnTi2O4 undergoes a structural transition into a polar P4_1 tetragonal structure and at further lower temperatures, around 45 K, the system undergoes a paramagnetic to ferrimagnetic transition. Magnetic superexchange interactions involving Mn and Ti spins and minimization of strain energy associated with co-operative Jahn-Teller distortions plays a critical role in stabilization of the unique tetramer-orbital ordered ground state which further gives rise to lattice chirality through subtle Ti-Ti bond-length modulations.

cond-mat.str-el

Structural response to the magnetic pre ordering in LiFeSi2O6

We investigate the temperature evolution of the structural parameters of potential ferrotoroidic LiFeSi2O6 compound across structural and magnetic phase transitions. The structural transition (TS)is around 220K and the paramagnetic to antiferromagnetic transition (TN) is around 18K. The lattice parameters exhibit unusual temperature dependence and based on its behaviour, the exper- imental results can be divided into 3 regions.In region I (300K to 240K), the cell parameters are mainly governed by mere thermal effect. As the compound enters region II (below 240K to 50K), the lattice parameters show non linear behaviour. In this region, the exchange pathways that lead to the magnetic interactions within and between the Fe-Fe chains do not show significant response.The region III (below 50K) is dominated by the magnetic contribution where we observe setting up of intra and inter-chain magnetic interaction. This behaviour is unlike other low dimensional com- pounds like Ca3Co2O6, Sr3NiRhO6, MnTiO3 etc. thereby suggesting the magnetism in LiFeSi2O6 is of three dimensional nature. The present results will be helpful in understanding the evolution of the spin rings that give rise to net toroidal moment and hence its multiferroic behaviour.

cond-mat.str-el

Direct evidence of the existence of Mn3+ ions in MnTiO3

We investigate the room temperature electronic properties of MnTiO3 synthesised by different preparation conditions. For this purpose, we prepared MnTiO3 under two different cooling rates, one is naturally cooled while the other is quenched in liq.nitrogen. The samples were studied using optical absorbance, photoemission spectroscopy and band structure calculations.We observe significant changes in the structural parameters as a result of quenching. Interestingly, in the parent compound, our combined core level, valence band and optical absorbance studies show the evidence of Mn existing in both 2+ and 3+ states. The fraction of Mn3+ ions has been found to increase on quenching. The increase in the fraction of the Mn3+ ions has been manifested (a) as slight enhancement in the intensity of the optical absorbance in the visible region.There occurs persistent photo-resistance when the incident light is terminated after shining; (b) in the behaviour of the features (close to fermi level) in the valence band spectra. Hence, the combined analysis of the core level, valence band and optical absorbance spectra suggest the charge carriers are hole like which further leads to the increase in the electrical conductivity of the quenched sample. The present results provide recipe to tune the optical absorption in the visible range for its applications in optical sensors, solar cell, etc.

cond-mat.str-el

Inverse photoemission spectroscopic studies on phase separated La$_{0.2}$Sr$_{0.8}$MnO$_{3}$

We have studied the temperature evolution of the inverse photoemission spectra of phase separated La$_{0.2}$Sr$_{0.8}$MnO$_{3}$. To identify the features in the room temperature experimental spectra, band structure calculations using Korringa-Kohn-Rostoker Green's function method were carried out. We find that the features generated by local moment disorder calculations give a better match with the experimental spectrum. In the insulating phase, we observed unusually an increased intensity at around the Fermi level. This puzzling behaviour is attributed to the shift in the chemical potential towards the conduction band. The present results clearly show the importance of unoccupied electronic states in better understanding of the phase separated systems.

cond-mat.str-el

Evidence of spin lattice coupling in MnTiO$_{3}$: an x-ray diffraction study

Here we investigate the temperature evolution of the structural parameters of a potential magnetoelectric material, MnTiO$_{3}$. The experimental results reveal interesting temperature dependence of the $c/a$ ratio and the Mn-O bonds which can be divided into three regions. In region I (300 K to 200 K), the above parameters are seen to decrease with decrease in temperature due to thermal effect. In the region II (200 K to 95 K), the decrement in the structural parameters are reduced due the competing intra layer antiferromagnetic interaction setting in $\sim$ 200 K. The $c/a$ ratio are seen to display a minima around 140 K. Below 140 K, the short Mn-O bonds increase suggesting the onset of inter layer antiferromagnetic interaction $\sim$ 100 K. In region III (95 K to 23 K), the antiferromagnetic interaction is fully established. The behaviour of the calculated Mn-O bonds based on first principle calculations are in line with the experimental results. This study demonstrates the importance of spin lattice coupling in understanding the magnetic properties of the compound which is expected to be helpful in revealing the origin of magnetically induced ferroelectricity.

cond-mat.str-el

Electronic structure of La(2)CoSi(3) - a non-Kondo analogue of a Kondo lattice, Ce(2)CoSi(3)

We study the electronic structure of a Pauli paramagnetic compound, La(2)CoSi(3) using photoemission spectroscopy and ab initio band structure calculations. Experimental valence band spectra exhibit signature of electron correlation induced feature around 2.5 eV - the correlation strength among Co 3d electrons is estimated to be close to 3 eV. The Co 2p core level spectra also exhibit correlation induced satellite features consistent with the scenario in the valence band spectra suggesting importance of conduction electron correlation in addition to the local moment in Kondo lattice systems. The La(2)CoSi(3) valence band spectra could be utilized to extract Ce 4f related spectral features and thus provide a good reference to study Kondo lattice systems in this class of materials. Temperature evolution of various core level spectra is found to be complex revealing deviations from a typical Fermi liquid behavior and emergence of distinct surface-bulk difference in the electronic structure at finite temperature.

cond-mat.str-el

Electronic structure of CaFe2As2

We investigate the electronic structure of CaFe$_2$As$_2$ using high resolution photoemission spectroscopy. Experimental results exhibit three energy bands crossing the Fermi level making hole pockets around the $Γ$-point. Temperature variation reveal a gradual shift of an energy band away from the Fermi level with the decrease in temperature in addition to the spin density wave (SDW) transition induced Fermi surface reconstruction of the second energy band across SDW transition temperature. The hole pocket in the former case eventually disappears at lower temperatures while the hole Fermi surface of the third energy band possessing finite $p$ orbital character survives till the lowest temperature studied. These results reveal signature of a complex charge redistribution among various energy bands as a function of temperature that might be associated to the exotic properties of this system.

cond-mat.supr-con

Electronic structure near quantum critical point

We studied the evolution of the electronic structure across the quantum critical point in V doped Cr employing high resolution photoemission spectroscopy. Experimental results exhibit signatures of pseudogap and orbital Kondo resonance peak at low temperatures for all the compositions studied suggesting a scenario of spin density wave quantum criticality corresponding to orbital Kondo effect. The pseudogap and the Kondo peak gradually reduces with V doping but remains finite at the quantum critical point indicating their relevance in widely discussed quantum phases in correlated electron systems. The spectral lineshape near the Fermi level exhibit (E_F - E)^{0.25} dependence evidencing deviation from Fermi liquid behavior.

cond-mat.str-el

Evidence of the influence of magnetism on pseudogap states in the high resolution spectra of EuFe$_2$As$_2$

Employing {\it state of the art} high resolution photoemission spectroscopy, we studied the temperature evolution of the electronic structure of EuFe$_2$As$_2$, an unique pnictide, where antiferromagnetism of 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 pseudogap-quasiparticle features having primarily As 4$p$ character and spin density wave transition induced band folding in the electronic structure. A weakly dispersing feature of dominant As 4$p$ character is discovered around 80 meV that becomes weaker in intensity below 20 K manifesting influence of antiferromagnetic order on conduction electrons. These results provide an evidence of a link between the pseudogap states and magnetism that could be revealed employing high resolutions.

cond-mat.supr-con

Importance of conduction electron correlation in a Kondo lattice, Ce2CoSi3

Kondo systems are usually described by the interaction of strong correlation induced local moment 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, Ce$_2$CoSi$_3$, using high resolution photoemission spectroscopy and {\it ab initio} band structure calculations, where Co 3$d$ electrons contribute in the conduction band. High energy resolution employed in the measurements helped to reveal signature of Ce 4$f$ states derived Kondo resonance feature at the Fermi level and dominance of Co 3$d$ contributions at higher binding energies in the conduction band. The line shape of the experimental Co 3$d$ 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 3$d$ electrons within the LDA+$U$ method leads to a better representation of experimental results. Signature of electron correlation induced satellite feature is also observed in the Co 2$p$ 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.

cond-mat.str-el

Spectral evolution in an insulator exhibiting linear specific heat

We investigate the spectral evolution of an antiferromagnetic insulator, La$_{0.2}$Sr$_{0.8}$MnO$_3$ exhibiting linear specific heat using state-of-the-art high resolution photoemission spectroscopy. Experimental spectral functions exhibit Fermi liquid like energy dependence at all the temperatures studied. Room temperature spectrum possess finite density of states at the Fermi level that vanishes generating a soft gap at about 260 K (the magnetic transition temperature). High resolution spectra reveal a hard gap in the magnetically ordered phase (C-type antiferromagnet). These results indicate signature of an amorphous phase coexisting with the long range ordered phase in these materials.

cond-mat.str-el

Importance of Co 3d electron correlation in a Ce-based Kondo lattice, Ce(2)CoSi(3)

We study the role of electron correlations among Co 3d electrons contributing to the conduction band of a Kondo lattice compound, Ce2CoSi3, using high resolution photoemission spectroscopy and ab initio band structure calculations. Experimental results reveal signature of Ce 4$f$ states derived Kondo resonance feature at the Fermi level and dominance of Co 3d contributions at higher binding energies in the valence band. The line shape of the experimental Co 3$d$ band is found to be significantly different from that obtained from the band structure calculations within the local density approximations. Consideration of electron-electron Coulomb repulsion among Co 3d electrons leads to a better representation of experimental results. The correlation strength among Co 3$d$ electrons is found to be about 3 eV. Signature of electron correlation induced satellite feature is also observed in the Co 2p core level spectrum. Thus, these results demonstrate the importance of the electron correlation among conduction electrons to derive the microscopic description of such Kondo systems.

cond-mat.str-el

An Automated Laboratory Laser Heating Arrangement for Materials Synthesis at High Temperatures and High Pressures

This paper describes the automation of a laser heating arrangement for synthesizing and studying materials at high pressures (up to ~ 1 Mbar) and high temperatures (up to ~ 5000 K). In this arrangement, a diamond anvil high-pressure cell (DAC) containing a microscopic sample of typical diameter ~50-100 micrometer, is mounted on a precision X-Y nanomotor stage that forms part of an IR laser heating optical assembly. Automation of this stage has been accomplished using a LabVIEW virtual instrument program to manipulate the X and Y stages using nanopositioning systems. This has a major feature of enabling a rastered heating of the sample over a user-defined circular area, without any operator intervention in addition to a virtual joystick to position the sample with respect to the laser spot. This auto-rastering feature has the advantage of offering uniform exposure of a circular area of the sample to the incident heating laser beam apart from drastic reduction in scan time compared to a manual scan. The diameter of the circle can be varied from a maximum of ~24 mm down to the focal spot size of the laser (~few micrometers), enabling thereby usage of the laser heating arrangement for heating microscopic samples under high-pressure in a DAC, as well as bulk samples at atmospheric pressure. Examples for both macro and micro scale automated laser-heating experiments have been presented. In particular, at the micro scale, auto-raster heated carbon samples at ~ 17 GPa and ~2000 K showed excellent signatures of diamond formation compared to manually raster heated samples, highlighting the unique advantage of auto-raster heating.

physics.ins-det

Electronic and structural transition in $La_{0.2} Sr_{0.8} Mn O_3$

We investigate the interplay of the electronic and structural transition in La$_{0.2}$Sr$_{0.8}$MnO$_{3}$. The transport and specific heat measurements exhibit unusual evolutions and signature of a first order phase transition around 265 K. Mn K-edge extended $x$-ray absorption fine structure results reveal distortion in the MnO$_6$ octahedra even in the cubic phase and a remarkable evolution of the distortion across the phase transition. These results manifest the importance of fluctuations in Mn 3$d$ orbital occupancy and disorder in their electronic properties, which may help in understanding the orbital and spin ordering proposed in these systems.

cond-mat.str-el

Doping and bond length contributions to Mn K-edge shift in La$_{1-x}$Sr$_x$MnO$_{3}$ and their correlation with electrical transport properties

The experimental Mn K-edge x-ray absorption spectra of La$_{1-x}$Sr$_x$MnO$_{3}$, $x$ = 0 - 0.7 are compared with the band structure calculations using spin polarized density functional theory. It is explicitly shown that there is a correspondence between the inflection point on the absorption edge and the centre of gravity of the unoccupied Mn 4$p$-band. This correspondence has been used to separate the doping and size contributions to edge shift due to variation in number of electrons in valence band and Mn-O bond lengths, respectively when Sr is doped into LaMnO$_3$. Such separation is helpful to find the localization behaviour of charge carriers and to understand the observed transport properties of these compounds.

cond-mat.str-el