arXiv subjects

Parasmani Rajput

Publications and source records attributed to Parasmani Rajput.

13 recordsLinked to original sources

arXiv2025

Local symmetry breaking and orbital glass behaviour in CoFe2O4

The structural distortions, orbital correlations, and electronic states in cobalt ferrite (CoFe2O4) were investigated using complementary characterisation techniques, including SR-XRD, HAXPES, XANES, EXAFS, and Raman spectroscopy. SR-XRD confirms phase purity and reveals a temperature-dependent superlattice reflection between 200 K and 100 K, consistent with the emergence of short-range orbital ordering driven by cooperative Jahn-Teller distortion (JTD). The disappearance of this feature below 100 K signals orbital freezing and the onset of a glass-like orbital state. HAXPES measurements show multiplet splitting and charge-transfer satellite features in the Co and Fe 2p core levels, indicating mixed valence states and strong electron correlations. XANES analysis reveals hybridized p-d states and local coordination distortions. Temperature-dependent EXAFS measurements indicate increasing local disorder-particularly in Fe-O and Fe-Fe octahedral bonds as evidenced by enhanced Debye-Waller factors. These distortions, attributed to cation redistribution and oxygen vacancies, are static and asymmetric, primarily affecting the octahedral sublattice. Notably, signatures of cooperative Jahn-Teller distortions emerge in the intermediate temperature range (200-100 K) and disappear upon further cooling. Raman spectroscopy further supports these findings, revealing phonon anomalies and enhanced spin-phonon coupling in the same temperature range. Magnetic measurements indicate spin reorientation and exchange interaction anomalies that align with the orbital behaviour. Together, these results hint at a frustrated orbital state in CoFe2O4 possibly involving cooperative Jahn-Teller distortions, disrupted long-range coherence, and orbital glass behaviour offering new insights into the coupling of orbital, spin, and lattice degrees of freedom in spinel systems.

cond-mat.str-el↗

arXiv2021

Synthesis and study of ScN thin films

To contemplate an alternative approach for the minimization of diffusion at high temperature depositions, present findings impart viability of room-temperature deposited reactively sputtered ScN thin film samples. The adopted room temperature route endows precise control over the $R_{N_2}$ flow for a methodical structural phase evolution from Sc$\to$ScN and probe the correlated physical aspects of the highly textured ScN samples. In the nitrided regime i.e. at $R_{N_2}$ = 2.5-100% flow, incorporation of unintentional oxygen defects were evidenced from surface sensitive soft x-ray absorption spectroscopy study, though less compared to their metal ($R_{N_2} = 0\%$) and interstitial ($R_{N_2} = 1.6\%$) counterparts, due to higher Gibb's free energy for Sc-O-N formation with no trace of ligand field splitting around the O K-edge spectra. To eradicate the sceptism of appearance of N K-edge (401.6 eV) and Sc L-edge (402.2 eV) absorption spectra adjacent to each other, the nascent Sc K-edge study has been adopted for the first time to validate complementary insight on the metrical parameters of the Sc-N system taken into consideration. Optical bandgaps of the polycrystalline ScN thin film samples were found to vary between 2.25-2.62 eV as obtained from the UV-Vis spectroscopy, whereas, the nano-indentation hardness and modulus of the as-deposited samples lie between 15-34GPa and 152-476GPa, respectively following a linearly increasing trend of resistance to plastic deformations. Besides, contrary to other early 3d transition metal nitrides (TiN, VN, CrN), a comprehensive comparison of noticeably large homogeneity range in Sc-N has been outlined to apprehend the minuscule lattice expansion over the large $R_{N_2}$ realm.

cond-mat.mtrl-sci↗

arXiv2021

d5-off-centering induced ferroelectric and magnetoelectric correlations in trirutile-Fe2TeO6

We present the rare existence of d5 off-centering, weak ferroelectric polarization and demonstrate its correlation with observed magnetoelectric (ME) properties in the G type (TN~210 K) antiferromagnet Fe2TeO6 (FTO) compound. The origin of ferroelectricity (FE) is associated with both lattice and asymmetric electron density distribution around the ion cores. ME coupling is observed in magnetic field-dependent polarization, ME voltage, and magnetostrain measurements. Short-range magnetic ordering due to intrabilayer dimeric exchange coupling via the double oxygen bridged Fe-O1-Fe pathway is proposed to play a dominating role to exhibit the negative nonlinear magnetic field dependent ME behavior at 300 K. Interbilayer exchange via Fe-O2-Fe pathways dominantly determines the hysteretic nonlinear magnetic field dependent ME response below TN. The observed nonlinear ME coupling signifies magnetoelasticity as manifested in the temperature and magnetic field-dependent strain measurement. Hence the rare existence of ferroelectricity and magnetoelectric coupling by d5 ion is presented in FTO.

cond-mat.mtrl-sci↗

arXiv2020

Strain Induced Relaxor-type Ferroelectricity Near Room Temperature in Delafossite CuCrO2

Polycrystalline samples of CuCrO2 were synthesized by solid state reaction method. Temperature dependent dielectric measurements, synchrotron x-ray diffraction (SXRD), pyroelectric current and Raman measurements have been performed on these samples. Evidences of the presence of relaxor type ferroelectricity, which otherwise have gone unnoticed in CuCrO2 system (a member of delafossite family) near room temperature, have been presented. Presence of broad maximum in dielectric permittivity and its frequency dispersion indicates relaxor-type ferroelectricity in CuCrO2 near room temperature. Careful analysis of temperature dependent SXRD data and Raman spectroscopic data indicates that the distorted CrO6 octahdera, is giving rise to strain in the sample. Due to this strain, polar regions are forming in an otherwise non-polar matrix, which is giving rise to relaxor type ferroelectricity in the sample. Regularization of CrO6 octahedra and disappearance of disorder induced peak in Raman spectra at high temperatures could be the reason behind observed dielectric anomaly in this sample. Present investigations propose that relaxor type ferroelectricity near room temperature is an inherent property of the CuCrO2 system, making it a fascinating material to be explored further.

cond-mat.mtrl-sci↗

arXiv2019

Radiation tolerance: Nano triumphs bulk

Materials are subjected to energetic particles in a number of radiation environments,and are hence prone to undesirable (radiation) damage.We report here the superiority of the nanocrystalline phase over bulk for radiation tolerance under simultaneous irradiation with high energy (electronic energy loss (Se) dominant) and low energy (nuclear energy loss (Sn) dominant) particles.Nano-crystalline yttria stabilized zirconia is found to exhibit lesser radiation damage (viz.degradation in crystallinity),when compared to its bulklike counterpart,against simultaneous irradiation with high energy 27 MeV Fe and low energy 900 keV I ions.This is interpreted within the framework of the thermal spike model after considering (i) the fact that there is essentially no spatial and time overlap between the damage events of the two simultaneous ion beams,and (ii) the influence of grain size on the radiation damage against separate Sn and Se.The present work besides being of keen interest for fundamental understanding of ion material interactions,also paves the way for the potential application of nanocrystalline materials in the nuclear industry where such simultaneous irradiations are encountered.

cond-mat.mtrl-sci↗

arXiv2019

Oxygen vacancy mediated cubic phase stabilization at room temperature in pure nano-crystalline Zirconia films: A combined experimental and first-principles based investigation

We report the formation of cubic phase, under ambient conditions, in thin films of Zirconia synthesized by electron beam evaporation technique. The stabilization of the cubic phase was achieved without the use of chemical stabilizers and/or concurrent ion beam bombardment. Films of two different thickness (660 nm, 140 nm) were deposited. The 660 nm and 140 nm films were found to be stoichiometric (ZrO2) and off-stoichiometric (ZrO1.7) respectively by Resonant Rutherford back-scattering spectroscopy. While the 660 nm as-deposited films were in the cubic phase, as indicated by X-ray diffraction and Raman spectroscopy measurements, the 140 nm as-deposited films were amorphous and the transformation to cubic phase was obtained after thermal annealing. Extended X-ray absorption fine structure measurements revealed the existence of Oxygen vacancies in the local structure surrounding Zirconium for all films. However, the amount of these Oxygen vacancies was found to be significantly higher for the amorphous films as compared to the films in the cubic phase (both 660 nm as-deposited and 140 nm annealed films). The cubic phase stabilization is explained on the basis of suppression of the soft X2- mode of vibration of the Oxygen sub-lattice due to the presence of the Oxygen vacancies. Our first-principles modeling under the framework of density functional theory shows that the cubic structure with Oxygen vacancies is indeed more stable at ambient conditions than its pristine (without vacancies) counterpart. The requirement of a critical amount of these vacancies for the stabilization of the cubic phase is also discussed.

cond-mat.mtrl-sci↗

arXiv2018

An experimental and Ab-initio study of Electronic and Magnetic properties of FeGa3

Electronic structure of FeGa3 has been studied using experiments and ab-initio calculations. Magnetization measurements show that FeGa3 is inherently diamagnetic in nature. Our studies indicate that the previously reported magnetic moment on the Fe atoms in FeGa3 is not an intrinsic property of FeGa3, but is primarily due to the presence of disorder, defects, grain boundaries etc that break the symmetry about the Fe dimers. Analysis of the results obtained from magnetic measurements, photoelectron spectroscopy, Fe K-edge X-ray absorption near edge spectroscopy and ab-initio calculations clearly indicates that, the effects of on-site Coulomb repulsion between the Fe 3d electrons do not play any role in determining the electronic and magnetic properties of FeGa3. Detailed analysis of results of single crystal and poycrystalline FeGa3, helps to resolve the discrepancy in the electronic and magnetic properties in FeGa3 existing in the literature, consistently.

cond-mat.mtrl-sci↗

arXiv2017

Search for Origin of Room Temperature Ferromagnetism Properties in Ni doped ZnO Nanostructure

The origin of room temperature (RT) ferromagnetism (FM) in Ni doped ZnO samples are systematically investigated through physical, optical, and magnetic properties of nanostructure, prepared by simple low-temperature wet chemical method. Reitveld refinement of X-ray diffraction pattern displays an increase in lattice parameters with strain relaxation and contraction in Zn/O occupancy ratio by means of Ni-doping. Similarly scanning electron microscope demonstrates modification in the morphology from nanorods to nanoflakes with Ni doping, suggests incorporation of Ni ions in ZnO. More interestingly, XANES (X-ray absorption near edge spectroscopy) measurements confirm that Ni is being incorporated in ZnO as Ni2+. EXAFS (Extended X-ray Absorption Fine Structure) analysis reveals that structural disorders near the Zn sites in the ZnO samples upsurges with increasing Ni concentration. Raman spectroscopy exhibits additional defect driven vibrational mode at 275 cm-1, appeared with Ni-doped sample only and the shift with broadening in 580 cm-1 peak, which manifests the presence of the oxygen vacancy (VO) related defects. Moreover, in photoluminescence (PL) spectra we observed peak appears at 524 nm, indicates the presence of singly ionized VO+, which may activate bound magnetic polarons (BMPs) in dilute magnetic semiconductors (DMSs). Magnetization measurements indicate weak ferromagnetism at RT, which rises with increasing Ni consolidation. It is therefore proposed that effect of the Ni-ions as well as the inherent exchange interactions rising from VO+ assist to produce BMPs, which are accountable for the RT-FM in Zn1-xNixO (0<x<0.125) system.

cond-mat.mtrl-sci↗

arXiv2017

Structure and Magnetization of Co4N Thin Film

In this work, we studied the local structure and the magnetization of Co4N thin films deposited by a reactive dc magnetron sputtering process. The interstitial incorporation of N atoms in a fcc Co lattice is expected to expand the structure and such expansion yields interesting magnetic properties characterized by a larger than Co magnetic moment and a very high value of spin polarization ratio in Co4N. By optimizing the growth conditions, we prepared Co4N film having lattice parameter close to its theoretically predicted value. The N concentration was measured using secondary ion mass spectroscopy. Detailed magnetization measurements using bulk magnetization method and polarized neutron reflectivity confirm that the magnetic moment of Co in Co4N is higher than that of Co.

cond-mat.mtrl-sci↗

arXiv2016

Optical bandgap and bowing parameter for Fe doped LaGaO3

The polycrystalline samples of LaGa1-xFexO3 have been prepared by standard solid state reaction route. The phase purity of the prepared samples is confirmed by powder xray diffraction experiments followed by Rietveld analysis. It has been observed that the variation of lattice parameters is governed by Vegards law. The optical band gap of these samples is estimated using diffuse reflectance analysis and it is observed that the optical gap systematically decreases with Fe doping from 3.62 eV and attains the saturation value of approximately 1.9 eV at x equal to 0.4. The value of the bowing parameter b for the prepared solid solution LaGa1-xFexO3 is estimated to be 3.8eV.The xray absorption near edge spectroscopy XANES suggests that the Fe is in mixed valence state in all prepared samples and these mixed states of Fe due to offstoichiometry acts like electron doping in LaGa1-xFexO3 and thereby results in the reduction in the effective band gap. Our results may be useful to design the LaGaO3based light emitting diodes and new generation of semiconductor photo-detectors.

cond-mat.str-el↗

arXiv2015

X-ray absorption (XANES) and photoelectron spectroscopy (XPS) of gamma irradiated Nd doped phosphate glass

This paper presents the X-ray absorption near edge structure (XANES) and X-ray photoelectron spectroscopic (XPS) studies of Nd doped phosphate glasses before and after gamma irradiation. The intensity and location of LIII edge white line peak of Nd are found to be dependent on the concentration of Nd as well as on the ratio of O/Nd in the glass matrix. The decrease in the peak intensity of white line of XANES spectra and asymmetry in the profile of Nd 3d5/2 peak of XPS after gamma irradiation clearly indicates that Nd3+ gets reduced to Nd2+ in the glass matrix, which increases with an increase in the doses of irradiation. Sharpening of Nd 3d5/2 XPS profile indicates about the deficiency of oxygen in the glass after gamma irradiation, which is supported by EDX measurement.

cond-mat.mtrl-sci↗

arXiv2014

A high resolution synchrotron x-ray powder diffraction study of the incommensurate modulation in the martensite phase of Ni2MnGa: Evidence for nearly 7M modulation and phason broadening

The modulated structure of the martensite phase of Ni2MnGa is revisited using high resolution synchrotron x-ray powder diffraction (SXRPD) measurements, which reveals higher order satellite reflections up to the 3rd order and phason broadening of the satellite peaks. The structure refinement, using the (3+1) dimensional superspace group approach, shows that the modulated structure of Ni2MnGa can be described by orthorhombic superspace group Immm(00$γ$)s00 with lattice parameters a= 4.21861(2) Å, b= 5.54696(3) Å, and c= 4.18763(2) Å and an incommensurate modulation wave vector q= 0.43160(3)c*= (3/7+$δ$)c*, where $δ$=0.00303(3) is the degree of incommensuration of the modulated structure. Additional satellite peak broadening, which could not be accounted for in terms of the anisotropic strain broadening based on a lattice parameter distribution , has been modeled in terms of phasons using fourth rank covariant strain tensor representation for incommensurate structures. The simulation of single crystal diffraction patterns from the refined structural parameters unambiguously reveals a rational approximant structure with 7M modulation. The inhomogeneous displacement of different atomic sites on account of incommensurate modulation and the presence of phason broadening clearly rule out the adaptive phase model proposed recently by Kaufmann et al.[1] and suggests that the modulation in Ni2MnGa originates from soft-mode phonons.

cond-mat.mtrl-sci↗

arXiv2014

Structural insight into $Co_{3-x}Mn_xTeO_6$; ($0 \lt x \le 2$) solid solutions using Synchrotron X-ray diffraction and XANES

Structural investigation on $Co_{3-x}Mn_xTeO_6$; ($0 \lt x \le 2$) solid solutions as a function of Mn concentration using Synchrotron X-ray diffraction (SXRD) and XANES measurements are presented. Phase diagram obtained from Rietveld Refinement on SXRD data as a function of Mn concentration indicates doping disproportionate mixing of both monoclinic (C2/c) and rhombohedral (R-3) structure (for $x \lt 0.5$) while only R-3 symmetry for $x \ge 0.5$. Furthermore, Rietveld analysis on SXRD data shows increase in lattice parameters and average transition metal oxygen (Co/Mn-O) bond lengths for $x \ge 0.5$. Co and Mn K-edge XANES spectra reveal that both Co and Mn are in mixed oxidation state of $Co^{2+}/Mn^{2+}$ and $Co^{3+}/Mn^{3+}$. Relative ratio of $Co^{3+}/Co^{2+}$ and $Mn^{3+}/Mn^{2+}$ using Linear combination fit (LCF) decrease with increasing $x$ for $x \ge 0.5$. These structural and spectroscopic evidences are used to provide possible interpretation of the reported observations of maximum Neel Temperature (TN) at $x ~\sim 0.5$ and enhancements of antiferro/ferro-magnetic interactions in $Co_{3-x}Mn_xTeO_6$ solid solutions.

cond-mat.mtrl-sci↗