arXiv subjects

D. M. Phase

Publications and source records attributed to D. M. Phase.

At least 19 recordsLinked to original sources

arXiv2023

Room temperature reversible colossal volto-magnetic effect in all-oxide metallicmagnet/topotactic-phase-transition material heterostructures

Multiferroic materials have undergone extensive research in the past two decades in an effort to produce a sizable room-temperature magneto-electric (ME) effect in either exclusive or composite materials for use in a variety of electronic or spintronic devices. These studies have looked into the ME effect by switching the electric polarization by the magnetic field or switching the magnetism by the electric field. Here, an innovative way is developed to knot the functional properties based on the tremendous modulation of electronics and magnetization by the electric field of the topotactic phase transitions (TPT) in heterostructures composed of metallic-magnet/TPT-material. It is divulged that application of a nominal potential difference of 2-3 Volts induces gigantic changes in magnetization by 100-250% leading to colossal Voltomagnetic effect, which would be tremendously beneficial for low-power consumption applications in spintronics. Switching electronics and magnetism by inducing TPT through applying an electric field requires much less energy, making such TPT-based systems promising for energy-efficient memory and logic applications as well as opening a plethora of tremendous opportunities for applications in different domains.

cond-mat.mtrl-sci↗

arXiv2022

Photosensitive SrMnO3

In recent years, photosensitive materials have been in huge demand because of their fascinating ability to convert absorbed photon energy to generate strain and henceforth tuning the physical properties. In this report we detect the photosensitive activity of SrMnO3. Using the power dependent and temperature dependent Raman study with different laser sources having wavelengths across the optical band gap of SrMnO3, we divulge the photosensitive character of SrMnO3 thin films. Upon laser light illumination, Raman modes soften and softening further increases with increase in laser power. Similar kind of mode variation is observed with increasing temperature at fixed laser power. XAS in presence of laser illumination, reveals the change in crystal field splitting associated with mode softening.

cond-mat.mtrl-sci↗

arXiv2022

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↗

arXiv2022

Exchange bias in Sm$ _{2} $NiMnO$ _{6}$/BaTiO$ _{3}$ ferromagnetic-diamagnetic heterostructure thin films

Exchange bias (EB) shifts are commonly reported for the ferromagnetic (FM)/antiferromagnetic (AFM) bilayer systems. While stoichiometric ordered Sm$_{2}$NiMnO$_{6}$ (SNMO) and BaTiO$_{3}$ (BTO) are known to possesses FM and diamagnetic orderings respectively, here we have demonstrated the cooling field dependent EB and training effects in epitaxial SNMO/BTO/SNMO (SBS) heterostructure thin films. The polarized Raman spectroscopy and magnetometric studies reveal the presence of anti-site cation disorders in background of ordered lattice in SNMO layers, which introduces Ni-O-Ni or Mn-O-Mn local AFM interactions in long range Ni-O-Mn FM ordered host matrix. We have also presented growth direction manipulation of the degree of cation disorders in the SNMO system. Polarization dependent X-ray absorption measurements, duly combined with configuration interaction simulations suggest charge transfer from Ni/Mn 3\textit{d} to Ti 3\textit{d} orbitals through O 2\textit{p} orbitals across the SNMO/BTO (SB) interfaces, which can induce magnetism in the BTO spacer layer. The observed exchange bias in SBS heterostructures is discussed considering the pinning of moments due to exchange coupling at SB (or BTO/SNMO) sandwich interface.

cond-mat.mtrl-sci↗

arXiv2022

Existence of inter coupled structural, electronic and magnetic states in Sm$ _{2} $NiMnO$ _{6} $ double perovskite

Coupling between different interactions allows to control physical aspects in multifunctional materials by perturbing any of the degrees of freedom. Here, we aim to probe the correlation among structural, electronic and magnetic observables of Sm$ _{2} $NiMnO$ _{6} $ ferromagnetic insulator double perovskite. Our employed methodology includes thermal evolution of synchrotron X-ray diffraction, near edge and extended edge hard X-ray absorption spectroscopy and bulk magnetometry. The magnetic ordering in SNMO adopts two transitions, at T$ _{C} $=159.6K due to ferromagnetic arrangement of Ni-Mn sublattice and at T$ _{d} $=34.1K because of anti-parallel alignment of polarized Sm paramagnetic moments with respect to Ni-Mn network. The global as well as local crystal structure of SNMO undergoes isostructural transitions across T$ _{C} $ and T$ _{d} $, observed by means of temperature dependent variation in Ni/Mn-O, Ni-Mn bonding characters and super exchange angle in Ni-O-Mn linkage. Hybridization between Ni, Mn 3\textit{d}, O 2\textit{p} electronic states is also modified in the vicinity of magnetic transition. On the other hand, the signature of Ni/Mn anti-site disorders are evidenced from local structure and magnetization analysis. The change in crystal environments governs the magnetic response by imposing alteration in metal - ligand orbital overlap. Utilizing these complimentary probes we have found that structural, electronic and magnetic states are inter-coupled in SNMO which makes it a potential platform for technological usage.

cond-mat.mtrl-sci↗

arXiv2022

Magnetic properties of disordered polycrystalline bulk Sm$ _{2} $NiMnO$ _{6} $ double perovskite

The structural, electronic and magnetic properties of anti-site disordered Sm$ _{2} $NiMnO$ _{6} $ double perovskite has been studied. RE$_{2}$NiMnO$_{6}$ (RE: rare-earth) ordered double perovskite is commonly believed to show two distinct magnetic phase transitions viz, paramagnetic to ferromagnetic (FM) transition at T = T$ _{C} $ due to Ni-O-Mn super exchange interaction and another transition at T = T$ _{d} $ due to coupling of RE spins with Ni-Mn network. In our present study, we have observed that the presence of intrinsic B-site disorder results in an additional antiferromagnetic (AFM) coupling, mediated via Ni-O-Ni and Mn-O-Mn local bond pairs. As a consequence, the magnetic behavior of SNMO comprises of co-existing FM-AFM phases, which are respectively governed by the anti-site ordered and disordered structures. Field dependent inverted cusp like trend in M(T) and two step reversible loop behavior in M(H) measurements indicate the presence of competing FM-AFM phases over a wide range of temperature values (T$ _{d} < $ T $ < $ T$ _{C} $).

cond-mat.mtrl-sci↗

arXiv2022

Microscopic insights of magnetism in Sm$ _{2} $NiMnO$ _{6} $ double perovskite

The functional characteristics of double perovskites with unique ferromagnetic-insulator ground state have been controversial due to the unavoidable presence of anti-site disorders (ASDs). Here, we aim to investigate the origin of magnetic ordering on local and global scales in Sm$_{2}$NiMnO$_{6}$ (SNMO) double perovskite system. Different calcination routes are exploited to generate different cation arrangements in SNMO and the corresponding magnetic configurations are examined using the high energy (E $ \sim $0.3 eV) `hot neutrons', which has helped to overcome Sm absorption as well as to record total (Bragg's+diffuse) scattering profiles with high momentum transfer (Q$ _{max} \sim $24 angstrom$ ^{-1} $). We have observed that the Ni-Mn sublattice adopts long range collinear ferromagnetic $ F_{x}F_{z} $ structure with commensurate $k$=(0, 0, 0) propagation vector, below ordering temperature T $ \lesssim $ 160 K, irrespective of variable ASD concentrations. In addition, the signatures indicating the antiparallel polarization of Sm paramagnetic moments with respect to Ni-Mn network, are noticed in the vicinity of anomalous magnetic transitions at T $ \lesssim $ 35 K. The real space pair distribution function calculations have provided a direct visualization of ASDs by means of broadening in Ni/Mn-Mn/Ni linkage. Employing the Reverse Monte Carlo approach on diffuse magnetic scattering profiles, we have observed the negative spin-spin correlation function which suggests the Ni-Ni antiferromagnetic exchange interactions ranging up to first nearest neighbor distance. These results confirm that the existence of ASDs in cation ordered host matrix leads to competing ferromagnetic-antiferromagnetic phases in a broad temperature range, which quantitatively governs the temperature dependent bulk magnetic observables of SNMO system.

cond-mat.mtrl-sci↗

arXiv2022

Mapping the magnetic state as a function of anti-site disorder in Sm$ _{2} $NiMnO$ _{6} $ double perovskite thin films

The predictability of any characteristic functional aspect in a double perovskite system has always been compromised by its strong dependence over the inevitably present anti-site disorders (ASD). Here, we aim to precisely map the quantitative and qualitative nature of ASD with the corresponding modifications in observables describing the magnetic and electronic state in epitaxial Sm$ _{2} $NiMnO$ _{6} $ (SNMO) double perovskite thin films. The concentration and distribution patterns of ASD are effectively controlled by optimizing growth conditions and estimated on both local and global scales utilizing extended X-ray absorption fine structure and bulk magnetometry. Depending upon the defect densities, the nature of disorder distribution can vary from homogeneous to partially segregated patches. Primarily, the effect of varying B-site cationic arrangement in SNMO is reflected as the competition of long range ferromagnetic (FM) and short scale antiferromagnetic (AFM) interactions originated from ordered Ni-O-Mn and disordered Ni-O-Ni or Mn-O-Mn bonds, respectively, which leads to systematic shift in magnetic transition temperature and drastic drop in saturation magnetization. In addition, we have observed that the gradual increment in density of ASD leads to significant deviation from uniaxial anisotropy character, reduction in anisotropy energy and enhancement of moment pinning efficiency. However, the observed signatures of $ Ni^{2+}+Mn^{4+} \longrightarrow Ni^{3+}+Mn^{3+} $ charge disproportionation is found to be independent of cation disorder densities. This work serves as a basic route-map to tune the characteristic magnetic anisotropy, magnetic phase transitions, and magnetization reversal mechanism by controlling ASD in a general double perovskite system.

cond-mat.mtrl-sci↗

arXiv2021

Spectroscopic comprehension of Mott-Hubbard insulator to negative charge transfer metal transition in LaNi_{x}V_{1-x}O_{3} thin films

The room temperature (300 K) electronic structure of pulsed laser deposited LaNi_{x}V_{1-x}O_{3} thin films have been demonstrated. The substitution of early-transition metal (TM) V in LaVO_{3} thin films with late-TM Ni leads to the decreasing in out-of-plane lattice parameter. Doping of Ni does not alter the formal valence state of Ni and V in LaNi_{x}V_{1-x}O_{3} thin films, divulging the absence of carrier doping into the system. The valence band spectrum is observed to comprise of incoherent structure owing to the localized V 3d band along with the coherent structure at Fermi level. With increase in Ni concentration, the weight of the coherent feature increases, which divulges its origin to the Ni 3d-O 2p hybridized band. The shift of Ni 3d-O 2p hybridized band towards higher energy in Ni doped LaVO_{3} films compared to the LaNiO_{3} film endorses the modification in ligand to metal charge transfer (CT) energy. The Ni doping in Mott-Hubbard insulator LaVO_{3} leads to the closure of Mott-Hubbard gap by building of spectral weight that provides the delocalized electrons for conduction. A transition from bandwidth control Mott-Hubbard insulator LaVO_{3} to negative CT metallicity character in LaNiO_{3} film is observed. The study reveals that unlike in Mott-Hubbard insulators where the strong Coulomb interaction between the 3d electrons decides the electronic structure of the system, CT energy can deliver an additional degree of freedom to optimize material properties in Ni doped LaVO_{3} films.

cond-mat.str-el↗

arXiv2020

Enhanced charge-transfer character in the monoclinic phase of Mott-insulator LaVO3 thin film

Electronic structure of pulsed laser deposited epitaxial LaVO3 (LVO) thin film grown on LaAlO3 (001) (LAO) substrate, has been studied at room temperature and at 130 K, which is below the structural (141 K) and magnetic transition temperatures (143 K) of single crystal LVO. Significant modification in spectral intensity, largely around the V 3d - O 2p hybridized region, is observed in valence band spectrum (VBS) of LVO film at 130 K. Resonant photoemission study at 130 K confirms the presence of charge transfer screened 3dnL (L: hole in the O 2p) final state along with the dominant 3dn-1 final state at 1.5 eV binding energy in the valence band. On the contrary, in the room temperature VBS dominant V 3d sates with only 3dn-1 kind final state is accentuated. To understand this difference, density functional theory (DFT) calculations are employed. The changes in crystal structure from room temperature orthorhombic (O-LVO) to low temperature monoclinic (M-LVO) symmetry leads to remarkable change in the electronic structure around the Fermi level, including transition from direct to indirect nature of band gap. Our calculations also confirm an enhanced O 2p character in the valence band edge of M-LVO that is hybridized with V 3d. These results are further corroborated with octahedral distortions associated with the structural transition.

cond-mat.str-el↗

arXiv2020

Synthesis and study of highly dense and smooth TiN thin films

This study aims towards a systematic reciprocity of the tunable synthesis parameters - partial pressure of N$_2$ gas, ion energy (\Ei) and Ti interface in TiN thin film samples deposited using ion beam sputtering at ambient temperature (300\,K). At the optimum partial pressure of N$_2$ gas, samples were prepared with or without Ti interface at \Ei~=~1.0 or 0.5\,keV. They were characterized using x-ray reflectivity (XRR) to deduce thickness, roughness and density. The roughness of TiN thin films was found to be below 1\,nm, when deposited at the lower \Ei~of 0.5\,keV and when interfaced with a layer of Ti. Under these conditions, the density of TiN sample reaches to 5.80($\pm$0.03)\,g~cm$^{-3}$, a value highest hitherto for any TiN sample. X-ray diffraction and electrical resistivity measurements were performed. It was found that the cumulative effect of the reduction in \Ei~from 1.0 to 0.5\,keV and the addition of Ti interface favors (111) oriented growth leading to dense and smooth TiN films and a substantial reduction in the electrical resistivity. The reduction in \Ei~has been attributed to the surface kinetics mechanism (simulated using SRIM) where the available energy of the sputtered species (\Esp) leaving the target at \Ei~= 0.5\,keV is the optimum value favoring the growth of defects free homogeneously distributed films. The electronic structure of samples was probed using N K-edge absorption spectroscopy and the information about the crystal field and spin-orbit splitting confirmed TiN phase formation. In essence, through this work, we demonstrate the role of \Esp~and Ti interface in achieving highly dense and smooth TiN thin films with low resistivity without the need of a high temperature or substrate biasing during the thin film deposition process.

cond-mat.mtrl-sci↗

arXiv2019

Magneto-dielectric coupling and non-ergodic electrical behaviour in hexagonal Sr0.6Ba0.4MnO3 via local strain driven magnetic ordering

The crystal structure of hexagonal-Sr0.6Ba0.4MnO3 allows various competing superexchange interactions, leading to intriguing magnetic properties. Local structural changes modify overlapping between Mn and oxygen ions with temperature. Calculations based on our model spin-Hamiltonian reveal that the dominant linear antiferromagnetic superexchange interaction between the oxygen-linked Mn4+ ions results in short range correlations (SRC), manifesting a smooth drop in magnetization below 325K. Dominance of superexchange interaction changes its allegiance towards the non-linear oxygen-linked Mn-O-Mn interactions, onsetting long-range correlations (LRC) below 225K. Below the SRC-LRC crossover temperature, electrical response arising from the interacting dipoles exhibits power-law divergent behaviour of relaxation time, upon cooling. Non-ergodic character of the dipole-cluster glass state is examined via the indispensable aging and rejuvenation effects, similar to the spin glasses. Competitive-frustration among spin-exchange and local-strain is reckoned as responsible for the electrical glass origin.

cond-mat.mtrl-sci↗

arXiv2019

Hexagonal Sr0.6Ba0.4MnO3: Spin and Dipole Coupling via Local Structure

Hexagonal Sr0.6Ba0.4MnO3 (SBMO) follows P63/mmc symmetry where MnO6 octahedra are both face-shared (Mn2O9 bi-octahedra) and corner-shared via oxygen anion. It undergoes ferroelectric (FE) and antiferromagnetic (AFM) orderings close to the room temperature. Magnetic properties appear to be governed by intricate exchange interactions among Mn4+ ions within and in adjacent Mn2O9 bi-octahedra, contingent upon the local structural changes. Calculations based on our model spin-Hamiltonian reveal that the dominant linear AFM fluctuations between the Mn4+ ions of two oxygen-linked bi-octahedra result in short range correlations, manifest as a smooth drop in magnetization below 325 K. Competition between spin-exchange and local-strain is reckoned as responsible for the atypical magneto-electricity, obtained near the room temperature.

cond-mat.mtrl-sci↗

arXiv2019

Influence of interface and microstructure on magnetization of epitaxial Fe4N thin film

Epitaxial Fe4N thin films grown on lattice-matched LaAlO3 (LAO) substrate using sputtering and molecular beam epitaxy techniques have been studied in this work. Within the sputtering process, films were grown with conventional direct current magnetron sputtering (dcMS) and for the first time, using a high power impulse magnetron sputtering (HiPIMS) process. Surface morphology and depth profile reveal that HiPIMS deposited film has the lowest roughness, the highest packing density and the sharpest interface. La from the LAO substrate and Fe from the film interdiffuse and forms an undesired interface spreading to an extent of about 10-20 nm. In the HiPIMS process, layer by layer type growth leads to a globular microstructure which restricts the extent of the interdiffused interface. Such substrate-film interactions and microstructure play a vital role in affecting the electronic hybridization and magnetic properties of Fe4N films. The magnetic moment (Ms) was compared using bulk, element-specific and magnetic depth profiling techniques. We found that Ms was the highest when the thickness of the interdiffused layer was lowest and only be achieved in the HiPIMS grown samples. Presence of small moment at the N site was also evidenced by element-specific x-ray circular dichroism measurement in HiPIMS grown sample. A large variation in the Ms values of Fe4N found in the experimental works carried out so far could be due to such interdiffused layer which is generally not expected to form in otherwise stable oxide substrate. In addition, a consequence of substrate-film interdiffusion and microstructure results in different kinds of different kind of magnetic anisotropies in films grown using different techniques.

cond-mat.mtrl-sci↗

arXiv2019

Tuning the Magnetic Ground State by Charge Transfer Energy in SrCoO2.5 via Strain Engineering

SrCoO2.5 (SCO) is a charge transfer insulator with 3d6 ground state configuration leading to antiferromagnetic nature. It is observed that substrate induced strain engineering modifies the ground state of SCO thin film with 3d7L (L:O-2p hole) configuration causing negative charge transfer energy.The consequent strong hybridization between O-2p and Co-3d bands causes a hole in O-2p band leading to hole mediated unconventional ferromagnetic ordering in SrCoO2.5 thin film. This opens up a new avenue to tune the electronic structure vis a vis magnetic property via strain engineering.

cond-mat.str-el↗

arXiv2019

Magnetism and structure of in-situ grown FeN films studied using N K-edge XAS and nuclear resonance scattering

We studied the structural and magnetic properties of \textit{in-situ} grown iron mononitride (FeN) thin films. Initial stages of film growth were trapped utilizing synchrotron based soft x-ray absorption near edge spectroscopy (XANES) at the N $K$-edge and nuclear resonant scattering (NRS). Films were grown using dc-magnetron sputtering, separately at the experimental stations of SXAS beamline (BL01, Indus 2) and NRS beamline (P01, Petra III). It was found that the initial stages of film growth differs from the bulk of it. Ultrathin FeN films, exhibited larger energy separation between the t$_{2g}$ and e$_g$ features and an intense e$_g$ feature in the N $K$-edge pattern. This indicates that a structural transition is taking place from the rock-slat (RS)-type FeN to zinc-blende(ZB)-type FeN when the thickness of films increases beyond 5\,nm. The behavior of such N $K$-edge features correlates very well with the emergence of a magnetic component appearing in the NRS pattern at 100\,K in ultrathin FeN films. Combining the \textit{in-situ} XANES and NRS measurements, it appears that initial FeN layers grow in RS-type structure having a magnetic ground state. Subsequently, the structure changes to ZB-type which is known to be non-magnetic. Observed results help in resolving the long standing debate about the structure and the magnetic ground state of FeN.

cond-mat.mtrl-sci↗

arXiv2019

Finding pathways for stoichiometric Co4N thin films

In this work, we studied the pathways for formation of stoichiometric \tcn~thin films. Polycrystalline and epitaxial \tcn~films were prepared using reactive direct current magnetron (dcMS) sputtering technique. A systematic variation in the substrate temperature (\Ts) during the dcMS process reveals that the lattice parameter (LP) decreases as \Ts~increases. We found that nearly stoichiometric \tcn~films can be obtained when \Ts~= 300\,K. However, they emerge from the transient state of Co target ($ϕ$3\,inch). By reducing the target size to $ϕ$1\,inch, now the \tcn~phase formation takes place from the metallic state of Co target. In this case, LP of \tcn~film comes out to be $\sim$99\p~of the value expected for \tcn. This is the largest value of LP found so far for \tcn. The pathways achieved for formation of polycrystalline \tcn~were adopted to grow an epitaxial \tcn~film, which shows four fold magnetic anisotropy in magneto-optic Kerr effect measurements. Detailed characterization using secondary ion mass spectroscopy indicates that N diffuses out when \Ts~is raised even to 400\,K. Measurement of electronic structure using x-ray photoelectron spectroscopy and x-ray absorption spectroscopy further confirms it. Magnetization measurements using bulk magnetization and polarized neutron reflectivity show that the saturation magnetization of stoichiometric \tcn~film is even larger than pure Co. Since all our measurements indicated that N could be diffusing out, when \tcn~films are grown at high \Ts, we did actual N self-diffusion measurements in a CoN sample and found that N self-diffusion was indeed substantially higher. The outcome of this work clearly shows that the \tcn~films grown prior to this work were always N deficient and the pathways for formation of a stoichiometric \tcn~have been achieved.

cond-mat.mtrl-sci↗

arXiv2019

Role of local short-scale correlations in the mechanism of negative magnetization

We elaborate here why the antiferromagnetically ordered GdCrO$_3$ responds in a diamagnetic way under certain conditions, by monitoring the evolution of the microscopic global and local magnetic phases. Using high energy $\sim$ 0.3 eV neutrons, the magnetic ordering is shown to adopt three distinct magnetic phases at different temperatures: G$_x^{Cr}$,A$_y^{Cr}$,F$_z^{Cr}$ below Néel temperature = 171 K; (F$_x^{Cr}$, C$_y^{Cr}$, G$_z^{Cr}$)$\bullet$( F$_x$$^{Gd}$,C$_y$$^{Gd}$) below 7 K and an intermediate phase for 7 K $ \le T \le$ 20 K in the vicinity of spin-reorientation phase transition. Although, bulk magnetometry reveals a huge negative magnetization (NM) in the terms of both magnitude and temperature range ( $M_{- max}$ ( 18 K)$\sim$ 35 $\times M_{+ max}$ (161 K), $ΔT \sim 110$ K in presence of $μ_0H$ = 0.01 T); the long-range magnetic structure and derived ordered moments are unable to explain the NM. Real-space analysis of the total (Bragg's + diffuse) scattering reveals significant magnetic correlations extending up to $\sim$ 9 $Å$. Accounting for these short-range correlations with a spin model reveals spin frustration in the S= 3 ground state, comprising competing first, second and third next nearest exchange interactions with values J$_1$ = 2.3 K, J$_2$ = -1.66 K and J$_3$ = 2.19 K in presence of internal field, governs the observance of NM in GdCrO$_{3}$.

cond-mat.mtrl-sci↗