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Dhananjai Pandey

Publications and source records attributed to Dhananjai Pandey.

At least 19 recordsLinked to original sources
arXiv2025

Local Symmetry Breaking in Skyrmion-Hosting Centrosymmetric Hexagonal Compounds

Dzyaloshinskii-Moriya interaction (DMI) plays a crucial role in stabilizing the exotic topologically stable skyrmion spin textures in the noncentrosymmetric crystals. The recent discovery of biskyrmions and skyrmions in the globally centrosymmetric crystals has raised debate about the role of the DMI in causing the spin textures, since DMI vanishes in such crystal structures. Theoretical studies, on the other hand, suggest non-vanishing DMI even if there is local inversion symmetry breaking in an otherwise globally centrosymmetric crystal structure. Motivated by such theoretical predictions, we present here the results of a systematic crystal structure study of two skyrmion-hosting Ni2In-type centrosymmetric hexagonal compounds, MnNiGa and MnPtGa, using the atomic pair distribution function (PDF) technique. Our result provides information about structural correlations in the short-range (SR), medium-range (MR) and long-range (LR) regimes simultaneously. The analysis of the experimental PDFs, obtained from high flux, high energy, and high Q synchrotron x-ray powder diffraction patterns, reveals that the local SR structure of both MnNiGa and MnPtGa compounds corresponds to the noncentrosymmetric trigonal space group P3m1, while the structure in the MR+LR regimes remains hexagonal in the centrosymmetric P63/mmc space group. These findings are also supported by theoretical DFT calculations. Our results, in conjunction with the previous theoretical predictions, provide a rationale for the genesis of skyrmions in centrosymmetric materials in terms of non-vanishing DMI due to local inversion symmetry breaking. We believe that our findings would encourage a systematic search of skyrmionic textures and other topological phenomena in a vast family of centrosymmetric materials.

cond-mat.mtrl-sci↗
arXiv2023

Evidence for Conical Magnetic Structure in M-type BaFe12O19 Hexaferrite: A Combined Single-Crystal XMCD and Neutron Diffraction Study

The magnetic ground state of BaFe12O19 (BFO) was investigated using X-ray absorption at 1.2 K and 1.5 K, respectively. The XMCD measurements on single-crystals of BFO in grazing incidence geometry reveal the canting of the spins away from the c-axis of the hexagonal unit cell. Single-crystal neutron diffraction studies reveal magnetic satellite peaks along the 00l reciprocal lattice row around the forbidden l = 2n +/- 1 positions confirming conical-type magnetic structure in the ground state of BFO. The observation of the conical magnetic structure of BFO opens the possibility of type-II multiferroicity in undoped BFO also.

cond-mat.mtrl-sci↗
arXiv2023

Evidence for reentrant quantum paraelectric state preceded by a multiglass phase with non-classical exponent and magnetodielectric coupling in SrFe12O19

Evidence for a re-entrant quantum paraelectric (QPE) state preceded by a dipole glass (DG) phase with a non-classical exponent in the quantum critical regime of SrFe12O19 is presented. It is shown that the DG transition is accompanied with a spin glass (SG) transition and presence of a biquadratic coupling of two diverse order parameter fields. Further, the ergodic symmetry breaking temperatures for the DG and SG transitions coincide (TDG ~ TSG) within +/- 1K suggesting that SrFe12O19 exhibits a canonical multiglass state. The stability of the dipole glass state is enhanced magnetically as evidenced by the increase in the freezing temperature with magnetic field (H). The re-entrant QPE state, on the other hand, is found to give way to another frequency dependent peak in the temperature dependence of dielectric constant, most likely a DG phase, at a constant H. Further, this transition is not linked to any magnetic transition in sharp contrast to the higher temperature multiglass transition. The transition temperature of this phase decreases with increasing magnetic field for a fixed frequency unlike the higher temperature DG transition. This raises the possibility of locating a quantum critical point (QCP) in this system at higher magnetic fields than that used in the present work. These results are discussed in the light of quantum critical models of multiferroic transitions. Our results highlight the need for more theoretical studies specific to multiferroic quantum criticality in a multiglass system.

cond-mat.str-el↗
arXiv2021

Robust evidence for the stabilization of the premartensite phase in Ni-Mn-In magnetic shape memory alloys by chemical pressure

The thermodynamic stability of the premartensite (PM) phase has been a topic of extensive investigation in shape memory alloys as it affects the main martensite phase transition and the related physical properties. In general, the PM phase is stable over a rather narrow temperature-composition range. We present here evidence for chemical pressure induced suppression of the main martensite transition and stabilization of the PM phase over a very wide temperature range from 300 K to around 5 K in a magnetic shape memory alloy (MSMA) Ni50Mn34In16 using magnetic susceptibility, synchrotron X-ray powder diffraction (SXRPD) studies and first-principles calculations. The ac-susceptibility studies show a highly skewed and smeared peak around 300 K without any further transition up to the lowest temperature of our measurement (5 K) for around 5% Al substitution. The temperature evolution of the SXRPD patterns confirms the appearance of the PM phase related satellite peaks at and below 300 K without any splitting of the main austenite (220) peak showing preserved cubic symmetry. This is in marked contrast to the temperature evolution of the SXRPD patterns of the martensite phase of the Al free as well as around 3% Al substituted compositions where the austenite (220) peak shows a clear splitting due to Bain distortion/symmetry breaking transition. Our theoretical calculations support the experimental findings and reveal that the substitution at the In site by a smaller size atom, like Al, can stabilize the PM phase with preserved cubic symmetry. Our results demonstrate that Al-substituted Ni-Mn-In MSMAs provide an ideal platform for investigating the physics of various phenomena related to the PM state.

cond-mat.mtrl-sci↗
arXiv2021

Evidence for Emergent Kagome Spin Configuration with Concomitant Transverse and Longitudinal Spin-Glass Freezing in the Chemically Ordered M-type Hexaferrite BaFe12O19

Frustration effects in magnetic systems have traditionally been investigated considering pre-existing site-disorder or lattice geometry of the high-temperature paramagnetic phase. We present here evidence for emergence of geometrical frustration as a function of temperature due to spin canting in the long-range ordered (LRO) ferrimagnetic (FMI) phase of BaFe12O19 (BFO), an M-type hexaferrite of enormous technological applications. Results of neutron scattering and magnetic susceptibility studies on BFO are presented to show for the first time the emergence of highly degenerate kagome spin configuration for the basal plane spin component of BFO with concomitant freezing of transverse and longitudinal components of the spins leading to two spin-glass transitions in coexistence with the LRO FMI phase. Our results mimic the theoretical predictions for concentrated Heisenberg systems even though the source of frustration in BFO is the geometry of the lattice and not site-disorder. We believe that our findings will stimulate theoretical studies to unravel the physics of spin-glass transitions in LRO systems due to emergent geometrical frustration, an aspect that has remained unexplored so far. We also believe that this work will encourage further experimental studies in search of low temperature spin-glass transition(s) in LRO phases of various hexaferrites and even other LRO magnetic compounds with spins arranged on triangular, pyrochlore and spinel lattices without any substitutional disorder.

cond-mat.mtrl-sci↗
arXiv2021

Precursor of the premartensite in Ni2MnGa magnetic shape memory alloy: A pair distribution function study

Precursor phenomena observed prior to the martensite phase transition plays a critical role towards the understanding of important technological properties of shape memory and magnetic shape memory alloys (MSMAs). The premartensite (PM) phase, considered as the precursor state of the martensite is proven to be a thermodynamically stable phase recently (Nature Commun. 8, 1006 (2017)), necessitates a critical investigation of precursor effects in these materials. We present here an evidence for the existence of a precursor state of the PM phase in Ni2MnGa MSMA using high energy synchrotron pair distribution function (PDF) study. The precursor state embedded within the austenite matrix in the short-range ordered (SRO) regime starting from far above the actual PM phase transition. The presence of such SRO precursor states of the PM phase produces strains which couple with the ferromagnetic (FM) order parameter around TC leading to first order character of the paramagnetic to FM phase transition.

cond-mat.mtrl-sci↗
arXiv2019

Evidence for pressure induced polarization rotation, octahedral tilting and reentrant ferroelectric phase in tetragonal (Pb0.5Bi0.5)(Ti0.5Fe0.5)O3

Despite the technological significance of the tetragonal PbTiO3 for the piezoelectric transducer industry, its high pressure behaviour is quite controversial as two entirely different scenarios, involving pressure induced (1) morphotropic phase boundary (MPB) like structural transition with concomitant rotation of the ferroelectric polarization vector and (2) antiferrodistortive (AFD) phase transition followed by emergence of a reentrant ferroelectric phase, have been proposed in recent theoretical and experimental studies. We have attempted to address these controversies through a high resolution synchrotron x-ray diffraction study of pressure induced phase transitions in the tetragonal phase of a modified PbTiO3 composition containing 50% BiFeO3, where BiFeO3 was added to enhance the AFD instability of PbTiO3. We present here the first experimental evidence for the presence of the characteristic superlattice reflections due to an AFD transition at a moderate pressure pc1 ~2.15 GPa in broad agreement with scenario (2), but the high pressure ferroelectric phase belongs to the monoclinic space group Cc, and not the tetragonal space group I4cm predicted under scenario (2), which permits the rotation of the ferroelectric polarization vector as per scenario (1). We show that the monoclinic distortion angle and ferroelectric polarization of the Cc phase initially decrease with increasing pressure for p < 7 GPa, but start increasing above pc2 ~ 7 GPa due to an isostructural Cc-I to Cc-II transition reminiscent of MA(apc > bpc ~ cpc) to MB(apc< bpc ~ cpc) transition predicted for MPB systems. We also show that octahedral tilting provides an efficient mechanism for accommodating pressure induced volume reduction for the stabilisation of the reentrant ferroelectric phase Cc-II.

cond-mat.mtrl-sci↗
arXiv2018

Evidence for superferrimagnetic clusters and spin-glass transition involving 4f Dy3+ spins in h-DyMnO3: A new twist to 4f Re3+ spin ordering in hexagonal manganites

The ferroelectric phase of the multiferroic hexagonal manganites (h-ReMnO3) has been reported to undergo a series of magnetic transitions involving long-range ordering/reorientation of 4fRe3+ and/or 3dMn3+ spins below room temperature. These transitions have attracted a lot of attention in recent years due to the geometrically frustrated nature of magnetic interactions. We have revisited these transitions in high quality single crystals of h-DyMnO3 using dc and ac susceptibility measurements as a function of temperature (T), magnetic field (H) and frequency (w) supplemented by specific heat measurements. Taking h-DyMnO3 as an example, we show that the Dy3+ spins below TN~68K are in a superferrimagnetic (SFIM) state whereas they undergo spin-glass (SG) transition below TDy3+~7K. Our observations demonstrate that neither the Néel transition at TN~68K nor the transition at TDy3+~7K is associated with long-range ordered states of Dy3+ spins as believed so far in the literature. The SG state of h-DyMnO3 is quite exotic as it occurs in an ordered compound purely due to geometrical frustration without any random disorder. Further, it shows an interesting crossover from de Almeida-Thouless type exponent (m=2/3) to Gabay-Toulouse type (m=2) with increasing field which cannot be explained in terms of the existing mean field theories of SG transition in Ising or Heisenberg systems but is expected for a vector X-Y SG system. Our observations call for a systematic reinvestigation of the nature of magnetic transitions involving Re3+ ions in other h-ReMnO3 also.

cond-mat.mtrl-sci↗
arXiv2018

Evidence for two spin-glass transitions with magnetoelastic and magnetoelectric couplings in the multiferroic (Bi$_{1-x}$Ba$_x$)(Fe$_{1-x}$Ti$_x$)O$_3$ system

For disordered Heisenberg systems with small single ion anisotropy, two spin glass transitions below the long range ordered phase transition temperature has been predicted theoretically for compositions close to the percolation threshold. Experimental verification of these predictions is still controversial for conventional spin glasses. We show that multiferroic spin glass systems can provide a unique platform for verifying these theoretical predictions via a study of change in magnetoelastic and magnetoelectric couplings, obtained from an analysis of diffraction data, at the spin glass transition temperatures. Results of macroscopic and microscopic (x-ray and neutron scattering) measurements are presented on disordered BiFeO3, a canonical Heisenberg system with small single ion anisotropy, which reveal appearance of two spin glass phases SG1 and SG2 in coexistence with the LRO phase below the A-T and G-T lines. It is shown that the temperature dependence of the integrated intensity of the antiferromagnetic peak shows dips with respect to the Brillouin function behaviour around the SG1 and SG2 transition temperatures. The ferroelectric polarisation changes significantly at the two spin glass transition temperatures. These results, obtained using microscopic techniques, clearly demonstrate that the SG1 and SG2 transitions occur on the same magnetic sublattice and are intrinsic to the system. We also construct a phase diagram showing all the magnetic phases in BF-xBT system. While our results on the two spin glass transitions support the theoretical predictions, it also raises several open questions which need to be addressed by revisiting the existing theories of spin glass transitions by taking into account the effect of magnetoelastic and magnetoelectric couplings as well as electromagnons.

cond-mat.mtrl-sci↗
arXiv2017

Origin of high piezoelectricity at the morphotropic phase boundary (MPB) in (Pb0.94Sr0.06)(ZrxTi1-x)O3

In this work, we address the issue of peaking of piezoelectric response at a particular composition in the morphotropic phase boundary (MPB) region of (Pb0.940Sr0.06)(ZrxTi1-x)O3 (PSZT) piezoelectric ceramics. We present results of synchrotron x-ray powder diffraction, dielectric, piezoelectric and sound velocity studies to critically examine the applicability of various models for the peaking of physical properties. It is shown that the models based on the concepts of phase coexistence, polarization rotation due to monoclinic structure, tricritical point and temperature dependent softening of elastic modulus may enhance the piezoelectric response in the MPB region in general but cannot explain its peaking at a specific composition. Our results reveal that the high value of piezoelectric response for the MPB compositions in PSZT at x=0.530 is due to the softening of the elastic modulus as a function of composition. The softening of elastic modulus facilitates the generation of large piezoelectric strain and polarization on approaching the MPB composition of x=0.530. This new finding based on the softening of elastic modulus may pave the way forward for discovering/designing new lead-free environmentally friendly piezoelectric materials and revolutionize the field of piezoelectric ceramics.

cond-mat.mtrl-sci↗
arXiv2017

Swift heavy ion irradiation induced structural phase transitions in BaTiO3: An in-situ x-ray diffraction study

There is considerable controversy about swift heavy ion (SHI) irradiation induced displacive phase transitions in thermally insulating oxides. We present here unambiguous evidence for tetragonal to monoclinic and rhombohedral to monoclinic phase transitions in BaTiO3 under swift heavy ion irradiation (120MeV 108Ag+9 ions) using in-situ x-ray powder diffraction (XRPD) studies. The anomalous splitting/broadening of 111/222pc, 200pc and 220pc pseudocubic peaks for fluences greater than 3*1012 ions/cm2 reveal structural changes before amorphization at higher fluences. Lebail analysis of XRPD profiles confirm that the monoclinic phase is of MA type in the Cm space group. Shear stress for the structural phase transition is estimated to be ~ 430MPa, which we believe is generated as a result of stopping of the SHI.

cond-mat.mtrl-sci↗
arXiv2016

Space group symmetries of the phases of (Pb0.94Sr0.06)(ZrxTi1-x)O3 across the antiferrodistortive phase transition in the composition range 0.620<x<0.940

The existing controversies about the space group symmetries of Pb(ZrxTi1-x)O3 (PZT) above and below antiferrodistortive (AFD) phase transition temperature (TAFD) in the Zr4+- rich (0.620<x<0.940) compositions are addressed using the results of dielectric, synchrotron x-ray powder diffraction (SXRPD) and neutron powder diffraction (NPD) studies. These compositions undergo an AFD phase transition above room temperature due to tilting of oxygen octahedral leading to a superlattice phase of PZT. We have substituted 6% Sr2+ at Pb2+-site to enhance the tilt angle and thereby the intensity of the superlattice peaks. The real and imaginary parts of complex dielectric permittivity have been used to locate the paraelectric to ferroelectric and ferroelectric to AFD phase transitions. Rietveld analysis of SXRPD and NPD profiles unambiguously reject the rhombohedral phases in R3c and R3m space groups below and above TAFD, respectively, with or without a coexisting monoclinic phase in Cm space group, and confirm that the true symmetries are monoclinic in Cc and Cm space groups below and above TAFD, respectively. Based on these and previous findings a phase diagram of PSZT for 0.40<x<0.90 showing stability fields of monoclinic Cc and monoclinic Cm, tetragonal P4mm and cubic Pm3m phases has also been presented.

cond-mat.mtrl-sci↗
arXiv2016

The Ground state of BiFeO3: Low temperature magnetic phase transitions revisited

Recent neutron diffraction and NMR studies suggest that the incommensurately modulated spin cycloid structure of BiFeO3 is stable down to 4.2 K, whereas DC [M(T)] and AC [\c{hi} (ω, T)] magnetization, and caloric studies have revealed several magnetic transitions including a spin glass transition around 25 K. The two sets of observations are irreconcilable and to settle this, it is important to first verify if the low temperature magnetic transitions are intrinsic to BiFeO3 or some of them are offshoots of oxygen vacancies and the associated redox reaction involving conversion of Fe3+ to Fe2+. We present here the results of M (T) and \c{hi} (ω, T) measurements on pure and 0.3 wt% MnO2 doped BiFeO3 samples in the 2 to 300 K temperature range. It is shown that MnO2 doping increases the resistivity of the samples by three orders of magnitude as a result of reduced oxygen vacancy concentration. A comparative study of the M (T) and AC \c{hi} (ω, T) results on two types of samples reveals that the transitions around 25 K, 110 K and 250 K may be intrinsic to BiFeO3. The widely reported transition at 50 K is argued to be defect induced, as it is absent in the doped samples. We also show that the spin glass transition temperature TSG is less than the spin glass freezing temperature (Tf), as expected for both canonical and cluster glasses, in marked contrast to an earlier report of TSG > Tf which is unphysical. We have also observed a cusp corresponding to the spin glass freezing at Tf in ZFC M (T) data not observed so far by previous workers. We argue that the ground state of BiFeO3 consists of the coexistence of the spin glass phase with the long range ordered AFM phase with a cycloidal spin structure.

cond-mat.mtrl-sci↗
arXiv2015

Premartensite to martensite transition and its implications on the origin of modulation in Ni2MnGa ferromagnetic shape memory alloy

We present here results of temperature dependent high resolution synchrotron x-ray powder diffraction study of sequence of phase transitions in Ni2MnGa. Our results show that the incommensurate martensite phase results from the incommensurate premartensite phase, and not from the austenite phase assumed in the adaptive phase model. The premartensite phase transforms to the martensite phase through a first order phase transition with coexistence of the two phases in a broad temperature interval (~40K), discontinuous change in the unit cell volume as also in the modulation wave vector across the transition temperature and considerable thermal hysteresis in the characteristic transition temperatures. The temperature variation of the modulation wave vector q shows smooth analytic behaviour with no evidence for any devilish plateau corresponding to an intermediate or ground state commensurate lock-in phases. The existence of the incommensurate 7M like modulated structure down to 5K suggests that the incommensurate 7M like modulation is the ground state of Ni2MnGa and not the Bain distorted tetragonal L10 phase or any other lock-in phase with a commensurate modulation. These findings can be explained within the framework of the soft phonon model.

cond-mat.mtrl-sci↗
arXiv2015

Residual stress induced stabilization of martensite phase and its effect on the magneto-structural transition in Mn rich Ni-Mn-In/Ga magnetic shape memory alloys

The irreversibility of the martensite transition in magnetic shape memory alloys (MSMAs) with respect to external magnetic field is one of the biggest challenges that limits their application as giant caloric materials. This transition is a magneto-structural transition that is accompanied with a steep drop in magnetization (i.e., 'delta M') around the martensite start temperature (Ms) due to the lower magnetization of the martensite phase. In this communication, we show that 'delta M' around Ms in Mn rich Ni-Mn based MSMAs gets suppressed by two orders of magnitude in crushed powders due to the stabilization of the martensite phase at temperatures well above the Ms and the austenite finish (Af) temperatures due to residual stresses. Analysis of the intensities and the FWHM of the x-ray powder diffraction patterns reveals stabilized martensite phase fractions as 97, 75 and 90% with corresponding residual microstrains as 5.4, 5.6 and 3% in crushed powders of the three different Mn rich Ni-Mn alloys, namely, Mn1.8Ni1.8In0.4, Mn1.75Ni1.25Ga and Mn1.9Ni1.1Ga, respectively. Even after annealing at 773 K, the residual stress stabilised martensite phase does not fully revert to the equilibrium cubic austenite phase as the magneto-structural transition is only partially restored with reduced value of 'delta M'. Our results have very significant bearing on application of such alloys as inverse magnetocaloric and barocaloric materials.

cond-mat.mtrl-sci↗
arXiv2014

Discovery of an isostructural phase transition within orthorhombic phase field of CaTiO3

Earths lower mantle extending from 670 to 2,990 km deep is predominantly composed of a perovskite-type (Mg,Fe)SiO3 phase1,2. The perovskite phase undergoes a structural phase transition to a post-perovskite phase responsible for D" layer seismic discontinuity2,3 at about 2690 km depth in the lowermost region of the lower mantle. However, structural basis of other seismic discontinuities occurring in the upper region of the lower mantle (700 km to 1,200 km deep) remains unexplained4-7, as no apparent change in the crystal symmetry of the orthorhombic perovskite phase has been reported5. We present here unambiguous evidence for a non-apparent isostructural phase transition8 in the stable orthorhombic perovskite phase of CaTiO3 which may have relevance to phase transitions in the perovskite phase of (Mg,Fe)SiO3 also, as both the compounds have similar structure, tolerance factor and thermochemical properties9-11. Our results are based on the analysis of neutron powder diffraction patterns using Rietveld and mode crystallography techniques and are supported by density functional and Landau theory calculations. The present results on CaTiO3 would encourage search for isostructural phase transition in the perovskite phase of (Mg,Fe)SiO3 that may provide clue to the unexplained geophysical phenomena in the upper part of the earths lower mantle.

cond-mat.mtrl-sci↗
arXiv2014

Extraordinary Tunability of the Superexchange Interactions in Nanoparticles of the Multiferroic 0.50BiFeO3-0.50PbTiO3

The coexistence and coupling of magnetic and ferroelectric orderings in single phase multiferroics has evinced enormous scientific interest as it involves breaking of time reversal and space inversion symmetries in the same material. The mutual controllability of the two diverse orderings in multiferroics has potential for developing new generation multifunctional sensor, actuator and data storage devices. We present here evidence for a new exotic facet of multiferroicity, whereby one can raise the strength of antiferromagnetic (AFM) superexchange interaction and hence tune the Néel temperature (TN) from ~120K in bulk to ~350K in 18nm size particles by tuning the ferroelectric distortion in the tetragonal phase of multiferroic (1-x)BiFeO3 -xPbTiO3 solid solutions . This observation is unique to multiferroics only as the TN in non-multiferroic AFM oxides decreases with particle size. Our results provide a scientific basis for designing room temperature single phase multiferroics, useful for making multifunctional device operating at room temperature.

cond-mat.mtrl-sci↗