arXiv subjects

Dinesh Kumar Shukla

Publications and source records attributed to Dinesh Kumar Shukla.

7 recordsLinked to original sources

arXiv2026

Optimization of magneto-electric properties in Lead-free (x)Co1.2Ti0.2Fe1.6O4 - (100-x)BaTiO3 based composites

This work presents a systematic study of lead-free multiferroic composites of (x)Co1.2Ti0.2Fe1.6O4 - (100-x)BaTiO3 (x = 10, 20, 30), which were synthesized by a solid-state reaction method to investigate the effects of composition and sintering temperature on their structural , electrical, magnetic, and magnetoelectric (ME) properties. X-ray diffraction along with Rietveld refinement confirms the coexistence of tetragonal BaTiO3 (BTO) and cubic spinel Co1.2Ti0.2Fe1.6O4 (CTFO) phases. Microstructural analysis shows that densification and grain growth are better at higher sintering temperatures, leading to better coupling between the two phases. Dielectric and ferroelectric studies indicate lossy polarization-electric field (P-E) behaviour due to leakage from the conductive phase, while magnetic properties show increased magnetization with increasing ferrite content. All composites exhibit ME coefficients, which depend on the composition and sintering conditions; the highest ME coefficient (~1.28 mV/cm.Oe) was observed for the 30CTFO - 70BTO composite sintered at 1200 °C. This improvement is due to the optimal balance between magnetostrictive and piezoelectric responses and improved interfacial strain transfer. These results demonstrate that simultaneous optimization of dopant-modified composition and sintering conditions is essential for achieving improved magnetoelectric coupling in bulk multiferroic composites. Moreover, the results demonstrate the potential of lead-free composites for multifunctional device applications in next-generation, low-power technologies, including high-density non-volatile memory (e.g. FeRAM/MRAM), magnetic field sensors, spintronic devices, and actuators.

cond-mat.mtrl-sci↗

arXiv2026

Visualization of Co 3d high- and low-spin states via valence electron density

Properties of trivalent cobalt oxides are governed by the spin and orbital states of Co3+ ions, which are strongly coupled to their local coordination environments and chemical bonding. However, direct real-space access to the electronic states has remained challenging. Here, we determine the Co 3d states in the quasi-one-dimensional cobalt oxide Ca3Co2O6 by combining synchrotron X-ray diffraction with valence electron density (VED) analysis based on core differential Fourier synthesis. The reconstructed VED reveals distinct anisotropic distributions at two crystallographically inequivalent Co sites with octahedral and trigonal-prismatic coordination geometries. The octahedral site exhibits a characteristic VED consistent with a low-spin configuration, whereas the trigonal-prismatic site shows pronounced anisotropy that cannot be described solely by crystal electric field (CEF) effects. Quantitative analysis demonstrates that this anisotropy originates from the interplay of CEF effects, spin-orbit coupling, and ligand-assisted 3d-4p hybridization, reflecting partially unquenched orbital angular momentum and its role in the Ising magnetism. These results establish a general framework for understanding site-dependent electronic structure and chemical bonding in transition-metal oxides through real-space VED analysis.

cond-mat.str-el↗

arXiv2025

Disorder mediated fully compensated ferrimagnetic spin-gapless semiconducting behaviour in Cr3Al Heusler alloy

Spin-gapless semiconductors (SGSs) that simultaneously host fully compensated ferrimagnetism are highly sought for energy-efficient and stray-field-free spintronic technologies, yet their realization in chemically disordered systems has remained elusive. Here, we demonstrate that the binary Heusler alloy Cr3Al despite adopting a fully A2-disordered structure exhibits a rare coexistence of SGS transport and a fully compensated ferrimagnetic (FCF) ground state. Single-crystalline and polycrystalline Cr3Al samples were synthesized, and comprehensive structural analyses using single crystal XRD, synchrotron powder XRD, and neutron powder diffraction reveal complete Cr/Al site mixing. Remarkably, this chemical disorder does not disrupt magnetic order; instead, magnetization, X-ray magnetic circular dichroism (XMCD), and temperature-dependent neutron diffraction establish a robust compensated ferrimagnetic state with a vanishingly small ordered moment of 0.1(1) muB/f.u and a high Curie temperature of 773(2) K. Electrical and thermal transport measurements uncover clear SGS characteristics, including weak temperature-dependent conductivity, very low Seebeck coefficients, and electron-hole compensated transport. Hall measurements show unusual temperature-dependent carrier concentrations consistent with disorder-modified electronic states. First-principles calculations on an A2-disordered SQS structure reproduce the experimentally observed negligibly small magnetization (0.0072 muB/f.u) and reveal a vanishing spin-up band gap unambiguously supporting SGS behavior driven by chemical disorder. Our results identify Cr3Al as the first experimentally verified A2-disordered Heusler alloy exhibiting both fully compensated ferrimagnetism and spin-gapless semiconducting transport, positioning it as a robust and disorder-tolerant platform for next-generation, high-temperature spintronic devices.

cond-mat.mtrl-sci↗

arXiv2025

Stranski-Krastanov Growth of Disordered ScNx Thin Films on MgO(100): Influence of Defect Densities on Electronic Structure and Transport Properties

We report a nascent real time Stranski-Krastanov growth of reactively sputtered ScNx thin films on MgO(100). The epitaxial growth was limited to 5 nm at a substrate temperature (Ts) of 25 C while the self-sustaining epitaxial nature along the [100] azimuth was retained up to 25 nm in Ts = 250 and 500 C samples due to enhanced adatom mobility. At Ts = 700 C, the film showed half order in-situ RHEED pattern, with forbidden (hkl) planes indicating N deficient hcp Sc-N phase. Presence of defect densities i.e., N vacancies and O interstitials leads to a disorder in ScNx system with weak localization effect and appearance of Raman relaxed first order transverse and longitudinal optical phonon modes and further leads to metal like Seebeck coefficient. Higher grain boundaries at Ts = 25 C and higher N out-diffusion at Ts = 700 C paves way for incorporation of higher oxygen interstitial in these samples.

cond-mat.mtrl-sci↗

arXiv2024

Size-induced Exchange Bias in Single-phase CoO Nanoparticles

We report exchange bias (EB) in single-phase CoO nanoparticles, where two magnetic phases naturally emerge as the crystallite size decreases from 34.6 to 10.8 nm. The Néel temperature (TN) associated with antiferromagnetic ordering decreases monotonically with the reduction in crystallite size, highlighting the significant influence of size effects. The 34.6 nm nanoparticles exhibit magnetization irreversibility between zero field cooled (ZFC) and field-cooled (FC) states below TN. This irreversibility appears well above TN with further reduction in size, resulting in the absence of true paramagnetic regime which indicates the occurrence of an additional magnetic phase. The frequency-dependent ac-susceptibility in 10.8 nm nanoparticles suggests slow dynamics of disordered surface spins above TN, coinciding with the establishment of long-range order in the core. The thermoremanent magnetization (TRM) and isothermoremanent magnetization (IRM) curves suggest a core-shell structure: the core is antiferromagnetic, and the shell consists of disordered surface spins causing ferromagnetic interaction. Hence, the exchange bias in these CoO nanoparticles results from the exchange coupling between an antiferromagnetic core and a disordered shell that exhibits unconventional surface spin characteristics.

cond-mat.mes-hall↗

arXiv2022

Coexistence of local structural heterogeneities and long-range ferroelectricity in Pb-free (1-x)Ba(Zr0.2Ti0.8)O3-x(Ba0.7Ca0.3)TiO3 ceramics

Environmentally benign (1-x)Ba(Ti$_{0.8}$Zr$_{0.2}$)O$_3$-x(Ba$_{0.7}$Ca$_{0.3}$)TiO$_3$ (BZT-BCT) ceramics are promising materials due to their remarkable high piezoresponse [Liu and Ren, Phys. Rev. Lett. \textbf{103}, 257602 (2009)]. In this Letter, by focusing on local and average structure in combination with macroscopic electromechanical and dielectric measurements we demonstrate the structure property relationship in the tetragonal BZT-BCT ceramic. During high-temperature cubic to tetragonal phase transformation, polar nanoregions are manifested through the spontaneous volume ferroelectrostriction at temperatures below $\sim$ 477 K. Temperature-dependent local structural investigations across the Zr K edge extended x-ray absorption fine structure spectroscopy reveal an anomalous collaboration between the ZrO$_{6}$ and TiO$_6$ octahedra. These octahedra compromise their individuality during polarization development. The presence of domains of submicron size embedded inside the macroscopic ferroelectric regions below T$_{m}$, as well as their hierarchical arrangement, is observed by piezo-response force microscopy. Effects of the existence of the structural/polar heterogeneities below T$_{m}$ are observed also when polarizibilities of the poled and the unpoled samples are compared; the poled sample is found to be more susceptible to the electric field. In addition, by using electric field dependent x-ray diffraction studies we also show that this ceramic under field exhibits reduction of tetragonal distortion, which is consistent with earlier reports.

cond-mat.mtrl-sci↗

arXiv2022

Monoclinic symmetry at the nanoscale in lead-free ferroelectric BaZr$_{x}$Ti$_{1-x}$O$_{3}$ ceramics

Local structural symmetries play a key role in the functionalities of ferroelectric materials and are often found different from average symmetry. Here, we study the real space nanoscale structure in Pb-free BaZr$_{x}$Ti$_{1-x}$O$_{3}$ (x $\leq$ 0.10) by pair distribution function measurements, complemented by transmission electron microscopy and x-ray diffraction. Our observations show existence of the rhombohedrally distorted unit cells; however, at intermediate length scales, at least up to 5 nm, there exist nano-scale correlated regions of monoclinic symmetry. This is complemented by the observation of curved frustrated nanodomains. Further, the average structure is found to have coexisting monoclinic and rhombohedral symmetries. Our observation of a two-phase ferroelectric state is in contrast to interferroelectric instabilities of conventional polymorphic phase boundaries reported for doped BaTiO$_{3}$.

cond-mat.mtrl-sci↗