arXiv subjects

Amritendu Roy

Publications and source records attributed to Amritendu Roy.

16 recordsLinked to original sources

arXiv2026

Beyond lead halide perovskites: visible light photovoltaics with phase engineered bismuth-based oxide double-perovskites, Bi2MCrO6 (M = Fe, Mn)

Lead poisoning and notorious ambient instability in lead-based halide perovskites pave the way for the exploration of alternative materials for affordable and efficient solar cell fabrication. An important prerequisite to this end is the optoelectronic evaluation of the proposed material. Here we report, optoelectronic characterization of Bi2FeCrO6 (BFCO) and Bi2MnCrO6 (BMCO) thin films vis-\`a-vis performance of photovoltaic cells. Solution-deposited thin films (350-450 nm) of the above compositions demonstrate a double-perovskite structure with monoclinic P21/c symmetry, albeit with mixed cation valences and deep-level defects. A thorough optoelectronic evaluation exhibits large optical absorption in the visible range ({\alpha} ~ 104 -105 cm-1), and high carrier density, ~1017-20 cm-3. Ultraviolet photoelectron spectroscopy measurement allowed determination of the positions of the band-edges (valence band maximum and conduction band minimum), required for the selection of carrier transport layers. In its first, BMCO-based FTO/SnO2/BMCO/Spiro-OMeTAD/Ag solar cell produced a maximum 3.56% conversion efficiency. Using numerical simulation, we predict that with suitable defect control, the above conversion efficiency can increase significantly.

cond-mat.mtrl-sci↗

arXiv2024

Itinerant magnetism vis-à-vis structural phases in AlCuFeMn multi-principal-component medium entropy alloy

The exploration of multi-principal-component alloys (MPCAs) as potential functional materials in research is still in its early phase, with most studies centred on their potential application as structural materials. Magnetic materials possessing superior performance characteristics are essential for functional applications. Experimental observations and ab-initio density functional theory calculations were used to design and investigate an MPCA, AlCuFeMn, based on the medium-entropy effect. This study examines the microstructure evolution, phase formation, and soft magnetic behaviour of a cast and annealed AlCuFeMn MPCA. We conducted first-principles density-functional-theory (DFT) calculations to explain a selected multi-phase alloy's atomic, electronic, and magnetic structures at absolute zero temperature to understand the experimental findings better. We verified the predictions based on DFT by comparing them with the experimental observations. Despite the emphasis on equimolar compositions, the findings and conclusions of this study can enhance phase prediction and magnetic characteristics in non-equimolar alloys.

cond-mat.mtrl-sci↗

arXiv2024

Understanding the phase stability in multi-principal-component AlCuFeMn alloy

Method(s) that can reliably predict phase evolution across thermodynamic parameter space, especially in complex systems are of critical significance in academia as well as in the manufacturing industry. In the present work, phase stability in equimolar AlCuFeMn multi-principal-component alloy (MPCA) was predicted using complementary first-principles density functional theory (DFT) calculations, and ab-initio molecular dynamics (AIMD) simulations. Temperature evolution of completely disordered, partially ordered, and completely ordered phases was examined based on Gibbs free energy. Configurational, electronic, vibrational, and lattice mismatch entropies were considered to compute the Gibbs free energy of the competing phases. Additionally, elemental segregation was studied using ab-initio molecular dynamics (AIMD). The predicted results at 300K align well with room-temperature experimental observations using x-ray diffraction, scanning and transmission electron microscopy on a sample prepared using commercially available pure elements. The adopted method could help in predicting plausible phases in other MPCA systems with complex phase stability.

cond-mat.mtrl-sci↗

arXiv2024

Improving the energy density and flexibility of PMN-0.3PT based piezoelectric generator by composite designing

Ceramics based piezoelectric generators are known for their high energy density and poor flexibility. In this work, v_r-PMN-0.3PT/PDMS 2-2 composite with optimum PMN-0.3PT content (v_r) was designed that demonstrated enhanced output energy density and superior mechanical flexibility under dynamic mechanical excitation. v_r-PMN-0.3PT/PDMS 2-2 composite with different PMN-PT reinforcement content (v_r) and two different reinforcement configurations were fabricated and characterized for effective electro-elastic properties and energy harvesting response. Parallelly, using the finite element method and analytical models, effective electromechanical properties were calculated. Composites with parallel connectivity of the reinforcement phase demonstrated enhanced piezoelectric charge coefficient even with low PMN-0.3PT content whereas the relative permittivity and elastic modulus exhibited a linearly increasing trend with reinforcement volume fraction. At a compressive load of 50 N and 5 Hz frequency, a piezoelectric generator (PG) based on a v_r = 0.2, v_r- PMN-0.3PT/PDMS 2-2 composite with parallel connectivity produced a maximum short-circuit current density of 69 nA/cm2 and an open-circuit electric field of 189 V/cm, translating to a maximum output power density of ~13 μW/cm3 higher than that of pristine PMN-0.3 PT based piezoelectric generator. Estimated mechanical flexibility was found to be ~53 % higher than that of pristine PMN-0.3PT.

physics.app-ph↗

arXiv2022

Room-temperature surface multiferroicity in Y$_2$NiMnO$_6$ nanorods

We report observation of surface-defect-induced room temperature multiferroicity - surface ferromagnetism ($M_S$ at 50 kOe $\sim$0.005 emu/g), ferroelectricity ($P_R$ $\sim$2 nC/cm$^2$), and significantly large magnetoelectric coupling (decrease in $P_R$ by $\sim$80\% under $\sim$15 kOe field) - in nanorods (diameter $\sim$100 nm) of double perovskite Y$_2$NiMnO$_6$ compound. In bulk form, this system exhibits multiferroicity only below its magnetic transition temperature $T_N$ $\approx$ 70 K. On the other hand, the oxygen vacancies, formed at the surface region (thickness $\sim$10 nm) of the nanorods, yield long-range magnetic order as well as ferroelectricity via Dzyloshinskii-Moriya exchange coupling interactions with strong Rashba spin-orbit coupling. Sharp drop in $P_R$ under magnetic field indicates strong cross-coupling between magnetism and ferroelectricity as well. Observation of room temperature magnetoelectric coupling in nanoscale for a compound which, in bulk form, exhibits multiferroicity only below 70 K underscores an alternative pathway for inducing magnetoelectric multiferroicity via surface defects and, thus, in line with magnetoelectric property observed, for example, in domain walls or boundaries or interfaces of heteroepitaxially grown thin films which do not exhibit such features in their bulk.

cond-mat.mtrl-sci↗

arXiv2022

Structural and electromechanical characterization of lead magnesium niobate-lead titanate (PMN-0.3PT) piezoceramic for energy harvesting applications

Efficient mechanical energy harvesting using the principle of piezoelectric effect demands specific material-property requirements. This includes a combination of large piezoelectric charge coefficient (dij), large elastic strain (εy), small elastic compliance (Sij), and small dielectric permittivity (\k{appa}ij). The present work undertakes structural, electrical, mechanical, and electromechanical characterization of pyrochlore-free lead magnesium niobate-lead titanate (1-x)[Pb(Mg(1/3)Nb(2/3)O3)]-xPbTiO3 at x = 0.3 or PMN-0.3PT, to estimate the above critical parameters for mechanical energy harvesting. Pyrochlore-free PMN-0.3PT ceramic with co-existing monoclinic (Pm and Cm) phases was synthesized using solid-state reaction method. Piezoelectric charge coefficient (d33), dielectric permittivity (\k{appa}33^T), elastic compliance (s33^E), and electromechanical coupling factor (k33), were estimated to be, 200 pC/N (approx), 1.06 (approx) x 10^-8 F/m, 13.16 (approx) x 10^-12 m2/N, and 0.54 (approx), respectively, using room temperature impedance measurement on a poled sample with specified dimensions (EN 50324-1:2002 and CEI/IEC 60483:1976). Polarization leakage due to transport of various charged defects was identified to be responsible for the reduced electromechanical properties compared to those reported for single crystals. Elastic strain (εy) vis-à-vis flexibility (fFOM) of the PMN-0.3PT was estimated to be 4.5 x 10-4. Energy harvesting under dynamic mechanical loading shows a maximum short-circuit current density, 95 nA/cm2, and an open-circuit electric field, 98 V/cm. With its impressive performance, PMN-0.3PT ceramic constitutes an important material for piezoelectric energy harvesting.

cond-mat.mtrl-sci↗

arXiv2019

Origin of Ferroelectricity in Orthorhombic LuFeO$_3$

We demonstrate that small but finite ferroelectric polarization ($\sim$0.01 $μ$C/cm$^2$) emerges in orthorhombic LuFeO$_3$ ($Pnma$) at $T_N$ ($\sim$600 K) because of commensurate (k = 0) and collinear magnetic structure. The synchrotron x-ray and neutron diffraction data suggest that the polarization could originate from enhanced bond covalency together with subtle contribution from lattice. The theoretical calculations indicate enhancement of bond covalency as well as the possibility of structural transition to the polar $Pna2_1$ phase below $T_N$. The $Pna2_1$ phase, in fact, is found to be energetically favorable below $T_N$ in orthorhombic LuFeO$_3$ ($albeit$ with very small energy difference) than in isostructural and nonferroelectric LaFeO$_3$ or NdFeO$_3$. Application of electric field induces finite piezostriction in LuFeO$_3$ via electrostriction resulting in clear domain contrast images in piezoresponse force microscopy.

cond-mat.str-el↗

arXiv2017

Phase partitioning in a novel near equi-atomic AlCuFeMn alloy

A novel low cost, near equi-atomic alloy comprising of Al, Cu, Fe and Mn is synthesized using arc-melting technique. The cast alloy possesses a dendritic microstructure where the dendrites consist of disordered FCC and ordered FCC phases. The inter-dendritic region is comprised of ordered FCC phase and spinodally decomposed BCC phases. A Cu segregation is observed in the inter-dendritic region while dendritic region is rich in Fe. The bulk hardness of the alloy is ~ 380 HV, indicating significant yield strength.

cond-mat.mtrl-sci↗

arXiv2016

Room temperature multiferroism in polycrystalline thin films of gallium ferrite

Sol-gel deposited (010) textured polycrystalline thin films of gallium ferrite (GaFeO3 or GFO) on n-Si(100) and Pt/Si(111) substrates are characterized for room temperature multiferroism. Structural characterization using X-ray diffraction and Raman spectroscopy confirms formation of single phase with nano-sized crystallites. Temperature dependent magnetization study demonstrates ferri to paramagnetic transition at ~300 K. Room temperature piezoresponse force microscopic analysis reveals local 180 degree phase switching of ferroelectric domains at very high coercive field EC, ~ 1350 kV/cm consistent with recent experimental and first-principles studies. Our study opens up possibility of integrating polycrystalline GFO in novel room temperature multiferroic devices.

cond-mat.mtrl-sci↗

arXiv2013

Optical Anisotropy in Bismuth Titanate: An Experimental and Theoretical Study

We report experimental and theoretical investigation of anisotropy in optical properties and their origin in the ferroelectric and paraelectric phases of bismuth titanate. Room temperature ellipsometric measurements performed on pulsed laser deposited bismuth titanate thin films of different orientations show anisotropy in the dielectric and optical constants, Subsequent first-principles calculations performed on the ground state structures of ferroelectric and high temperature paraelectric phases of bismuth titanate show that the material demonstrates anisotropic optical behavior in both ferroelectric and paraelectric phases. We further show that O 2p to Ti 3d transition is the primary origin of optical activity of the material while optical anisotropy results from the asymmetrically oriented Ti-O bonds in TiO6 octehdra in the unit cell.

cond-mat.mtrl-sci↗

arXiv2013

Room Temperature Nanoscale Ferroelectricity in Magnetoelectric GaFeO3 Epitaxial Thin Films

We demonstrate room temperature ferroelectricity in the epitaxial thin films of magnetoelectric GaFeO3. Piezo-force measurements show a 180o phase shift of piezoresponse upon switching the electric field indicating nanoscale ferroelectricity in epitaxial thin films of gallium ferrite. Further, temperature dependent impedance analysis with and without the presence of an external magnetic field clearly reveals a pronounced magneto-dielectric effect across the magnetic transition temperature. In addition, our first principles calculations show that Fe ions are not only responsible for ferrimagnetism as observed earlier, but also give rise to the observed ferroelectricity, making GFO an unique single phase multiferroic.

cond-mat.mtrl-sci↗

arXiv2013

Engineering Polarization Rotation in Ferroelectric Bismuth Titanate

Here, we report a combined experimental-theoretical study showing that collective application of rare earth doping on A-site and epitaxial strain to ferroelectric bismuth titanate does not lead to a very large c-axis polarization as reported previously. Further first principles calculations based on the examination of polarization tensor suggest that simultaneous Bi and Ti site doping could result in moderate polarization along c-axis of bismuth titanate which is typically a preferential axis of film growth and thus enabling c axis oriented films to have appreciable polarization. This approach could also be applicable to other ferroic oxides where one can correlate the doping, epitaxial strain, and polarization to design materials compositions resulting in epitaxial films grown along desired directions yielding substantial polarization.

cond-mat.mtrl-sci↗

arXiv2012

Effect of Site-disorder, Off-stoichiometry and Epitaxial Strain on the Optical Properties of Magnetoelectric Gallium Ferrite

We present a combined experimental-theoretical study demonstrating the role of site disorder, off-stoichiometry and strain on the optical behavior of magnetoelectric gallium ferrite. Optical properties such as band-gap, refractive indices and dielectric constants were experimentally obtained by performing ellipsometric studies over the energy range 0.8 eV to 4.2 eV on pulsed laser deposited epitaxial thin films of stoichiometric gallium ferrite with b-axis orientation and the data was compared with theoretical results. Calculations on the ground state structure show that the optical activity in GaFeO3 arises primarily from O2p-Fe3d transitions. Further, inclusion of site disorder and epitaxial strain in the ground state structure significantly improves the agreement between the theory and the room temperature experimental data substantiating the presence of site-disorder in the experimentally derived strained GaFeO3 films at room temperature. We attribute the modification of the ground state optical behavior upon inclusion of site disorder to the corresponding changes in the electronic band structure, especially in Fe3d states leading to a lowered band-gap of the material.

cond-mat.mtrl-sci↗

arXiv2011

First Principle Study of Magnetism and Magneto-structural Coupling in Gallium Ferrite

We report a first-principles study of the magnetic properties, site disorder and magneto-structural coupling in multiferroic gallium ferrite (GFO) using local spin density approximation (LSDA+U) of density functional theory. The calculations of the ground state A-type antiferromagnetic structure predict magnetic moments consistent with the experiments whilst consideration of spin-orbit coupling yields a net orbital moment of ~ 0.025 Bohr magneton/Fe site also in good accordance with the experiments. We find that though site disorder is not spontaneous in the ground state, interchange between Fe2 and Ga2 sites is most favored in the disordered state. The results show that ferrimagnetism in GFO is due to Ga-Fe site disordering such that Fe spins at Ga1 and Ga2 sites are antiferromagnetically aligned while maintaining ferromagnetic coupling between Fe spins at Ga1 and Fe1 sites as well as between Fe spins at Ga2 and Fe2 sites. The effect of spin configuration on the structural distortion clearly indicates presence of magneto-structural coupling in GFO.

cond-mat.mtrl-sci↗

arXiv2011

Electronic Structures, Born Effective Charges and Spontaneous Polarization in Magnetoelectric Gallium Ferrite

We present a theoretical study of the structure-property correlation in gallium ferrite, based on the first principles calculations followed by a subsequent comparison with the experiments. Local spin density approximation (LSDA+U) of the density functional theory has been used to calculate the ground state structure, electronic band structure, density of states and Born effective charges. Calculations reveal that the ground state structure is orthorhombic Pc21n having A-type antiferromagnetic spin configuration, with lattice parameters matching well with those obtained experimentally. Plots of partial density of states of constituent ions exhibit noticeable hybridization of Fe 3d, Ga 4s, Ga 4p and O 2p states. However, the calculated charge density and electron localization function show largely ionic character of the Ga/Fe-O bonds which is also supported by lack of any significant anomaly in the calculated Born effective charges with respect to the corresponding nominal ionic charges. The calculations show a spontaneous polarization of ~ 59 microC/cm^2 along b-axis which is largely due to asymmetrically placed Ga1, Fe1, O1, O2 and O6 ions.

cond-mat.mtrl-sci↗

arXiv2010

First-Principles Calculation of Born Effective Charges and Spontaneous Polarization of Ferroelectric Bismuth Titanate

In this study, we present the results of our first-principles calculations of the band structure, density of states and the Born effective charge tensors for the ferroelectric (ground state B1a1) and paraelectric (I4/mmm) phases of bismuth titanate. The calculations are done using the generalized gradient approximation (GGA) as well as the local density approximation (LDA) of the density functional theory. In contrast to the literature, our calculations on B1a1 structure using GGA and LDA yield smaller indirect band gaps as compared to the direct band gaps, in agreement with the experimental data. The density of states shows considerable hybridization among Ti 3d, Bi 6p and O 2p states indicating covalent nature of the bonds leading to the ferroelectric instability. The Born effective charge tensors of the constituent ions for the ground state (B1a1) and paraelectric (I4/mmm) structures were calculated using the Berry phase method. This is followed by the calculation of the spontaneous polarization for the ferroelectric B1a1 phase using the Born effective charge tensors of the individual ions. The calculated value for the spontaneous polarization of ferroelectric bismuth titanate using different Born effective charges was found to be in the range of 55+/-13 $μ$C/cm2 in comparison to the reported experimental value of (50+/-10 $μ$C/cm2) for single crystals. The origin of ferroelectricity is attributed to the relatively large displacements of those oxygen ions in the TiO6 octahedra that lie along the a-axis of the bismuth titanate crystal.

cond-mat.mtrl-sci↗