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Ram Janay Choudhary

Publications and source records attributed to Ram Janay Choudhary.

10 recordsLinked to original sources

Unraveling the temperature-responsive charge-disproportionation in BaBiO$_3$

This study shows that the charge disproportionation at the Bi site in BaBiO$_3$ alters as a function of temperature. Decreasing the temperature from 300K down to 160K leads to a significant modification of the density of states corresponding to the Bi-O hybridized band near the Fermi level (E$_\text{F}$). This modification indicates reduction of Bi 6$sp$ - O 2$p$ hybridization and O 2$p$ spectral weight near E$_\text{F}$. The strong decrement of covalency at lower temperatures is accompanied by a decrement in O 2$p$ hole density due to possible charge transfer from Bi 6$s$ to the O 2$p$ band. Bi-charge state analysis from Bi-4$f$ core-level spectra showed that at 300K, $δ$ (charge difference between alternate Bi sites) value in 4$\pmδ$ is much less than at 160K, which reveals the transition towards the ionic nature of CD or static CD in BBO at low temperature. On the other hand, O 1$s$ core-level spectra displayed an asymmetric shape, and temperature-dependent modifications of the asymmetric shape and intensity have been observed. This highlights the significant influence of the O 2$p$ band hole on the dynamical CD at the Bi site.

cond-mat.mtrl-sci↗

Competing s-p and p-p fluctuations in charge-disproportionation of BaBiO3

Here we investigate the mechanism of charge-disproportionation (CD) in BaBiO3 (BBO) using density functional theory under different crystal symmetries and by employing strain as an external perturbation. The competition between Bi 6sp-O 2p (s-p) and O 2p-O 2p (p-p) charge-fluctuations decides the electronic ground state, charge-disproportionation and bond-disproportionation (BD) in BBO. An extended Hubbard Hamiltonian involving onsite (U) and long-range (V) coulomb repulsions is also employed to ascertain the microscopic conditions for the formation of the lone-pair on bismuth site. A strong tensile strain increases p-p fluctuation and enhances negative-charge transfer (CT) character, while strong compressive strain favors s-p fluctuation leading to more positive-CT character. Bulk BBO is at the verge of positive and negative-CT regimes.

cond-mat.mtrl-sci↗

Light-induced giant and persistent changes in the converse magnetoelastic effects in Ni/BaTiO3 multiferroic heterostructure

Magnetoelastic and magnetoelectric coupling in the artificial multiferroic heterostructures facilitate valuable features for device applications such as magnetic field sensors and electric write magnetic-read memory devices. In a ferromagnetic/ferroelectric heterostructures, the strain mediated coupling exploits piezoelectricity/electrostriction in ferroelectric phase and magnetostriction/piezomagnetism in ferromagnetic phase. Such verity of these combined effect can be manipulated by an external perturbation, such as electric field, temperature or magnetic field. Here, we demonstrate the remote-controlled tunability of these effects under the visible, coherent and polarized light. The combined surface and bulk magnetic study of domain-correlated Ni/BaTiO3 heterostructure reveals that the system is strong sensitive about the light illumination via the combined effect of converse piezoelectric, magnetoelastic coupling and converse magnetostriction. Well-defined ferroelastic domain structure is fully transferred from a tetragonal ferroelectric to magnetostrictive layer via interface strain transfer during the film growth. The visible light illumination is used to manipulate the original ferromagnetic microstructure by the light-induced domain wall motion in ferroelectric, consequently the domain wall motion in the ferromagnetic layer. Our findings mimic the attractive remote-controlled ferroelectric random-access memory write and magnetic random-access memory read application scenarios, hence, can be proven as a novel perspective for room temperature device applications.

cond-mat.mtrl-sci↗

Strain and electric field control of magnetic and electrical transport properties in a magneto-elastically coupled Fe3O4/BaTiO3(001) heterostructure

We present a study of the control of electric field induced strain on the magnetic and electrical transport properties in a magneto-elastically coupled artificial multiferroic Fe3O4/BaTiO3 heterostructure. In this Fe3O4/BaTiO3 heterostructure, the Fe3O4 thin film is epitaxially grown in the form of bilateral domains, analogous to a-c stripe domains of the underlying BaTiO3(001) substrate. By in-situ electric field dependent magnetization measurements, we demonstrate the extrinsic control of the magnetic anisotropy and the characteristic Verwey metal-insulator transition of the epitaxial Fe3O4 thin film in a wide temperature range between 20-300 K, via strain mediated converse magnetoelectric coupling. In addition, we observe strain induced modulations in the magnetic and electrical transport properties of the Fe3O4 thin film across the thermally driven intrinsic ferroelectric and structural phase transitions of the BaTiO3 substrate. In-situ electric field dependent Raman measurements reveal that the electric field does not significantly modify the anti-phase boundary defects in the Fe3O4 thin film once it is thermodynamically stable after deposition and that the modification of the magnetic properties is mainly caused by strain induced lattice distortions and magnetic anisotropy. These results provide a framework to realize electrical control of the magnetization in a classical highly correlated transition metal oxide.

cond-mat.mtrl-sci↗

Role of local structural distortions on the origin of j=1/2 pseudo-spin state in sodium iridate

Na2IrO3 (NIO) is known to be a spin-orbit (SO) driven j=1/2 pseudo-spin Mott-Hubbard (M-H) insulator. However, the microscopic origin of the pseudo-spin state and the role of local structural distortions have not been clearly understood. Using a combination of theoretical calculations and x-ray spectroscopy, we show that the energetics in the vicinity of Fermi level (EF) is governed by SO interactions, electron correlation and local octahedral distortions. Contrary to the earlier understanding, here we show that the j=3/2 and 1/2 pseudo-spin states have admixture of both t2g and eg characters due to local structural distortion. Reduction of local octahedral symmetry also enables Ir 5d- O2p hybridization around the EF resulting in a M-H insulator with enhanced charge transfer character. The possibility of Slater insulator phase is also ruled out by a combination of absence of room temperature DoS in valence band spectra, calculated moments and temperature dependent magnetization measurements.

cond-mat.mtrl-sci↗

Synthesis and characterization of vertically aligned La0.7Sr0.3MnO3:NiO nanocomposite thin films for spintronic applications

The microstructures and interfaces of two-phase vertically aligned nanocomposite (VAN) thin films play a key role in the design of spintronic device architectures and their multifunctional properties. Here, we show how the microstructures in self-assembled VAN thin films of La0.7Sr0.3MnO3:NiO (LSMO:NiO) can be effectively tuned from nano-granular to nano-columnar, and to nano-maze by controlling the number of laser shots from the two constituent phase targets in the pulsed laser deposition (PLD) film growth. The observed microstructural induced strain is found to significantly enhance the magnetoresistance in a very broad temperature range between 10-240 K and to modulate the in-plane exchange bias (EB), with the largest EB value observed in the maximally strained heterostructures. Most interestingly, a unique perpendicular exchange bias (PEB) effect is also observed for these heterostructures with an enhanced PEB field of up to 230 Oe. X-ray magnetic circular dichroism and training effect measurements demonstrate that the observed EB is disorder-induced and arises due to the pinning of NiO uncompensated moments at the disordered interface which is ferromagnetically coupled with LSMO. Furthermore, systematic changes in the electronic structure across the vertical interface related to a variation of the Mn3+/Mn4+ content arise as a consequence of out-of-plane tensile strain.

cond-mat.str-el↗

Engineering room-temperature multiferroicity in Bi and Fe codoped BaTiO3

Fe doping into BaTiO3, stabilizes the paraelectric hexagonal phase in place of the ferroelectric tetragonal one [P. Pal et al. Phys. Rev. B, 101, 064409 (2020)]. We show that simultaneous doping of Bi along with Fe into BaTiO3 effectively enhances the magnetoelectric (ME) multiferroic response (both ferromagnetism and ferroelectricity) at room-temperature, through careful tuning of Fe valency along with the controlled-recovery of ferroelectric-tetragonal phase. We also report systematic increase in large dielectric constant values as well as reduction in loss tangent values with relatively moderate temperature variation of dielectric constant around room-temperature with increasing Bi doping content in Ba1-xBixTi0.9Fe0.1O3 (0<x<0.1), which makes the higher Bi-Fe codoped sample (x=0.08) promising for the use as room-temperature high-k dielectric material. Interestingly, x=0.08 (Bi-Fe codoped) sample is not only found to be ferroelectrically (~20 times) and ferromagnetically (~6 times) stronger than x=0 (only Fe-doped) at room temperature, but also observed to be better insulating (larger bandgap) with indirect signatures of larger ME coupling as indicated from anomalous reduction of magnetic coercive field with decreasing temperature. Thus, room-temperature ME multiferroicity has been engineered in Bi and Fe codoped BTO (BaTiO3) compounds.

cond-mat.mtrl-sci↗

Coexisting 1T/2H polymorphs, reentrant resistivity behavior, and charge distribution in MoS2-hBN 2D/2D composite thin films

In view of their immensely intriguing properties, two dimensional materials are being intensely researched in search of novel phenomena and diverse application interests, however, studies on the realization of nanocomposites in the application-worthy thin-film platform are rare. Here we have grown MoS2-hBN composite thin films on different substrates by the pulsed laser deposition technique and made comparative studies with the pristine MoS2 and hBN films. The Raman, XPS and HRTEM confirm the concomitant presence of both the 1T (conducting) and 2H (semiconducting) polymorphs of MoS2 in the composite film. Interestingly, a peculiar reentrant semiconductor-metal-insulator transition is seen in the composite film which is absent in the MoS2 film, and it correlates well with the signatures of phonon softening seen in temperature-dependent Raman spectroscopy. Furthermore, electrostatic force microscopy reveals the presence of three distinct regions (metallic, semiconducting, and insulating) in the composite film with differing contact potentials and enhanced propensity for charge transfer with respect to pristine MoS2. A triboelectric nanogenerator device containing biphasic composite film as an electron acceptor exhibits more than twofold (sixfold) enhancement in peak-to-peak output voltage as compared to the pristine MoS2 (hBN) film. These observations bring out the potential of nanocomposite thin films for unfolding emergent phenomena and technological applications.

cond-mat.mtrl-sci↗

Electronic structure depiction of magnetic origin in BaTiO$_{3-δ}$ thin film: A combined experimental and first-principles based investigation

With the motive of unraveling the origin of native vacancy induced magnetization in ferroelectric perovskite oxide systems, here we explore the consequences of electronic structure modification in magnetic ordering of oxygen deficient epitaxial BaTiO$_{3-δ}$ thin films. Our adapted methodology employs state-of-the-art experimental approaches viz. photo-emission, photo-absorption spectroscopies, magnetometric measurements duly combined with first principles based theoretical methods within the frame work of density functional theory (DFT and DFT+\textit{U}) calculations. Oxygen vacancy (O$ _{V} $) is observed leading partial population of Ti 3\textit{d} (t$_{2g}$), which induces defect state in electronic structure near the Fermi level and reduces the band gap. The oxygen deficient BaTiO$_{2.75} $ film reveals Mott-Hubbard insulator characteristic, in contrast to the band gap insulating nature of the stoichiometric BaTiO$ _{3}$. The observed magnetic ordering is attributed to the asymmetric distribution of spin polarized charge density in the vicinity of O$ _{V} $ site which originates unequal magnetic moment values at first and second nearest neighboring Ti sites, respectively. Hereby, we present an exclusive method for maneuvering the band gap and on-site electron correlation energy with consequences on magnetic properties of BaTiO$_{3-δ}$ system, which can open a gateway for designing novel single phase multiferroic system.

cond-mat.mtrl-sci↗

Quantum Paraelectric Glass State in SrCu3Ti4O12

Magnetic and dielectric studies of SrCu3Ti4O12 carried out over 5-300K confirm antiferromagnetic (AFM) ordering of Cu-spins at TN =23K. Dielectric constant ε' measured across 1Hz-1MHz signifies quantum paraelectric character, Barrett-fittable almost down to TN. Competition of athermal fluctuations and the literature-reported magneto-phonon-softening near TN manifests a maiden quantum paraelectric glass (QPG) state. Emergent AFM-field tunes the otherwise quantum ordering (at absolute-zero) of the dipoles to finite-temperature kinetic glass transition; spectral dispersion of dielectric constant unambiguously manifested and characterized. Vogel-Fulcher glass-kinetics parameterization sets the almost relaxation-free QPG state in SrCu3Ti4O12 apart from an emergent scaling-class, to which typical ferroelectric relaxors belong.

cond-mat.mtrl-sci↗