arXiv subjects

Dhananjai Pandey

Publications and source records attributed to Dhananjai Pandey.

At least 37 records · Page 2Linked to original sources

arXiv2014

A high resolution synchrotron x-ray powder diffraction study of the incommensurate modulation in the martensite phase of Ni2MnGa: Evidence for nearly 7M modulation and phason broadening

The modulated structure of the martensite phase of Ni2MnGa is revisited using high resolution synchrotron x-ray powder diffraction (SXRPD) measurements, which reveals higher order satellite reflections up to the 3rd order and phason broadening of the satellite peaks. The structure refinement, using the (3+1) dimensional superspace group approach, shows that the modulated structure of Ni2MnGa can be described by orthorhombic superspace group Immm(00$γ$)s00 with lattice parameters a= 4.21861(2) Å, b= 5.54696(3) Å, and c= 4.18763(2) Å and an incommensurate modulation wave vector q= 0.43160(3)c*= (3/7+$δ$)c*, where $δ$=0.00303(3) is the degree of incommensuration of the modulated structure. Additional satellite peak broadening, which could not be accounted for in terms of the anisotropic strain broadening based on a lattice parameter distribution , has been modeled in terms of phasons using fourth rank covariant strain tensor representation for incommensurate structures. The simulation of single crystal diffraction patterns from the refined structural parameters unambiguously reveals a rational approximant structure with 7M modulation. The inhomogeneous displacement of different atomic sites on account of incommensurate modulation and the presence of phason broadening clearly rule out the adaptive phase model proposed recently by Kaufmann et al.[1] and suggests that the modulation in Ni2MnGa originates from soft-mode phonons.

cond-mat.mtrl-sci↗

arXiv2014

Ground state of (Pb0.94Sr0.06)(Zr0.530Ti0.470)O3 in the morphotropic phase boundary region: Evidence for a monoclinic Cc space group

The antiferrodistortive (AFD) phase transition for a pseudotetragonal composition of Pb(Zr0.530Ti0.470)O3 (PZT) doped with 6% Sr has been investigated using sound velocity (4 to 320K), high resolution synchrotron X-ray powder diffraction (100 to 800K) and high resolution as well as high flux neutron powder diffraction measurements (4K) to settle the existing controversies about the true ground state of PZT in the morphotropic phase boundary (MPB) region. The multiplet character of the neutron diffraction profiles of (3/2 1/2 1/2)pc (pseudocubic or pc indices) and (3/2 3/2 1/2)pc superlattice peaks, appearing below the AFD transition temperature, rules out the rhombohedral R3c space group. The true ground state is confirmed to be monoclinic in the Cc space group in agreement with the predictions of the first principles calculations and earlier findings for pure PZT in the MPB region. 6% Sr2+ substitution and the use of high wavelength (λ=2.44Å) neutrons have played key role in settling the existing controversies about the true ground state of PZT in the MPB region.

cond-mat.mtrl-sci↗

arXiv2014

Antiferrodistortive Phase Transition in Pseudorhombohedral (Pb0.94Sr0.06)(Zr0.550Ti0.450)O3 : A Combined Synchrotron x-ray and Neutron Powder Diffraction Study

The controversies about the structure of the true ground state of pseudorhombohedral compositions of Pb(ZrxTi1-x)O3 (PZT) are addressed using a 6% Sr2+ substituted sample with x=0.550. Sound velocity measurements reveal a phase transition at Tc~279K. The temperature dependence of FWHM of (h00)pc peaks and the unit cell volume also show anomalies around 279K even though there is no indication of any change of space group in the synchrotron X-ray powder diffraction (SXRD) patterns. The neutron powder diffraction patterns reveal appearance of superlattice peaks below Tc~279K confirming the existence of an antiferrodistortive phase transition. The Rietveld analysis of the room temperature and low temperature SXRD data below Tc shows that the structure corresponds to single monoclinic phase in the Cm space group while the analysis of neutron powder diffraction data reveals that the structure of the ground state phase below Tc corresponds to the Cc space group. Our analysis shows that the structural models for the ground state phase based on R3c space group with or without the coexistence of the room temperature monoclinic phase in the Cm space group can be rejected.

cond-mat.mtrl-sci↗

arXiv2014

Evidence for a tricritical point coinciding with the triple point in (Pb0.94Sr0.06)(ZrxTi1-x)O3 : A combined synchrotron x-ray diffraction, dielectric and Landau theory study

We present here results of high resolution synchrotron x-ray diffraction (SXRD) and dielectric studies in conjunction with Landau theory considerations on (Pb0.94Sr0.06)(ZrxTi1-x)O3 compositions in the vicinity of the morphotropic phase boundary (MPB) to find evidence for the flattening of the free energy surface at the MPB proposed in recent ab-initio studies on strongly piezoelectric ceramics. SXRD results reveal that the tetragonal and pseudorhombohedral monoclinic compositions with x=0.515 and 0.550 transform directly into the cubic paraelectric phase, whereas for 0.520<x<0.545, the pseudotetragonal as well as pseudorhombohedral monoclinic compositions first transform to the tetragonal phase and then to the cubic phase. Our results reveal the existence of a triple point at x~0.550. It is shown that the tetragonal to cubic transition, irrespective of the composition, upto x~0.545 is accompanied with a discontinuous change in the unit cell volume and thermal hysteresis confirming first order nature of this transition. The pseudorhombohedral monoclinic composition for x=0.550, on the other hand, transforms directly into the cubic phase in a second order manner. Our experimental results thus reveal a crossover from first order to second order phase transition through a tricritical point around x=0.550. Landau theory calculations also confirm gradual flattening of the free energy surface on approaching the tricritical composition x=0.550. We conclude that the triple point in the PZT phase diagram is indeed a tricritical point.

cond-mat.mtrl-sci↗

arXiv2014

Confirmation of the monoclinic Cc space group for the ground state phase of Pb(Zr0.525Ti0.475)O3 (PZT525): A Combined Synchrotron X-Ray and Neutron Powder Diffraction Study

The low temperature antiferrodistortive phase transition in a pseudo-tetragonal composition of PZT with x=0.525 is investigated through a combined synchrotron x-ray and neutron powder diffraction study. It is shown that the superlattice peaks cannot be correctly accounted for in the Rietveld refinement using R3c or R3c+Cm structural models, whereas the Cc space group gives excellent fits to the superlattice peaks as well as to the perovskite peaks. This settles at rest the existing controversies about the structure of the ground state phase of PZT in the MPB region.

cond-mat.mtrl-sci↗

arXiv2010

Absence of Morphotropic Phase Boundary Effects in BiFeO3-PbTiO3 Thin Films Grown via a Chemical Multilayer Deposition Method

Here, we report the unusual behaviour shown by the (BiFeO3)1-x-(PbTiO3)x (BF-xPT) films prepared using a multilayer deposition approach by chemical solution deposition method. Thin film samples of various compositions were prepared by depositing several bilayers of BF and PT precursors by varying the BF or PT layer thicknesses. X-ray diffraction showed that final samples of all compositions show mixing of the two compounds resulting in a single phase mixture, also confirmed by transmission electron microscopy. In contrast to bulk equilibrium compositions, our samples show a monoclinic (MA type) structure suggesting disappearance of morphotropic phase boundary (MPB) about x = 0.30 as observed in the bulk. This is accompanied by the lack of any enhancement of remnant polarization at MPB as shown by the ferroelectric measurements. Magnetic measurements show that the magnetization of the samples increases with increasing BF content. Significant magnetization of the samples indicates melting of spin spirals in the BF-xPT arising from random distribution of iron atoms across the film. Absence of Fe2+ ions in the films was corroborated by X-ray photoelectron spectroscopy measurements. The results illustrate that used thin film processing methodology significantly changes the structural evolution in contrast to predictions from the equilibrium phase diagram as well as modify the functional characteristics of BP-xPT system dramatically.

cond-mat.mtrl-sci↗

arXiv2010

Structural Changes and Ferroelectric Properties of BiFeO 3 -PbTiO 3 Thin Films Grown via a Chemical Multilayer Deposition Method

Thin films of (1-x)BiFeO 3 -xPbTiO 3 (BF-xPT) with x ~ 0.60 were fabricated on Pt/Si substrates by chemical solution deposition of precursor BF and PT layers alternately in three different multilayer configurations. These multilayer deposited precursor films upon annealing at 700°C in nitrogen show pure perovskite phase formation. In contrast to the equilibrium tetragonal structure for the overall molar composition of BF:PT::40:60, we find monoclinic structured BF-xPT phase of M A type. Piezo-force microscopy confirmed ferroelectric switching in the films and revealed different normal and lateral domain distributions in the samples. Room temperature electrical measurements show good quality ferroelectric hysteresis loops with remanent polarization, Pr, of up to 18 μC/cm 2 and leakage currents as low as 10 -7 A/cm 2 .

cond-mat.mtrl-sci↗

arXiv2009

Evidence for First Order Cubic Paraelectric to Rhombohedral Ferroelectric Phase Transition in 0.8BiFeO3-0.2Pb(Fe1/2Nb1/2)O3

The current controversies about the existence of an intermediate 'beta' phase of BiFeO_3 and the high temperature paraelectric 'gamma' phase are resolved by studying the sequence of ferroic transitions in 0.8BiFeO_3-0.2Pb(Fe_1/2Nb_1/2)O_3 (BF-0.2PFN) with lowered transition temperature. It is shown that the room temperature ferroelectric phase of 0.8BF-0.2PFN in the R3c space group transforms to the paraelectric/paraelastic cubic (Pm-3m) phase directly without any intermediate 'beta' phase reported in the literature. This transition is of first order type as confirmed by the coexistence of R3c and Pm-3m phases over a 100K range and a discontinuous change in the unit cell volume.

cond-mat.mtrl-sci↗

arXiv2008

Direct Evidence for Multiferroic Magnetoelectric Coupling in 0.9BiFeO3-0.1BaTiO3

Magnetic, dielectric and calorimetric studies on 0.9BiFeO3-0.1BaTiO3 indicate strong magnetoelectric coupling. XRD studies reveal a very remarkable change in the rhombohedral distortion angle and a significant shift in the atomic positions at the magnetic Tc due to an isostructural phase transition. The calculated polarization using Rietveld refined atomic positions scales linearly with magnetization. Our results provide the first unambiguous evidence for magnetoelectric coupling of intrinsic multiferroic origin in a BiFeO3 based system.

cond-mat.mtrl-sci↗

arXiv2008

Structural Basis for the Anomalously Low Spontaneous Polarisation Values of the Polar Phase of Sr1-xCaxTiO3 (x=0.02, 0.04): Evidence for a Ferrielectric Ordering

Full pattern Le-Bail refinement using x-ray powder diffraction profiles of Sr1-xCaxTiO3 for x=0.02, 0.04 in the temperature range 12 to 300 K reveals anomalies in the unit cell parameters at 170, 225 K due to an antiferrodistortive (cubic to tetragonal I4/mcm) phase transition and at ~32, ~34 K due to a transition to a polar phase (tetragonal I4/mcm to orthorhombic Ic2m), respectively. The lower transition temperatures obtained by us are in excellent agreement with those reported on the basis of the dielectric studies by Bednorz and Muller, [10] who attributed these to ferroelectric transition. Rietveld analysis of the diffraction profiles of the polar phase reveals off-centre displacements of both Sr2+/Ca2+ and Ti4+ ions in the X-Y plane along <110> pseudocubic directions, in agreement with the experimentally reported direction of easy polarization by Bednorz and Muller, but the resulting dipole moments are shown to be ferrielectrically coupled in the neighbouring (001) planes along the [001] direction leading to anomalously low values of the spontaneous polarization at 12K.

cond-mat.mtrl-sci↗

arXiv2008

Existence of Large Room Temperature Ferroelectricity in Chemical Solution Grown PbTiO3 Buffered (BiFeO3)1-x-(PbTiO3)x Films on Pt/Si Substrates

Here, we report the existence of large remnant polarization and dielectric constant in PbTiO3 buffered polycrystalline (BiFeO_3)_{1-x} (PbTiO_3)_x thin films of composition x = 0.25, 0.30 and 0.35 around the morphotropic phase boundary. The films were deposited by chemical solution deposition on platinized silicon substrates. Films reveal a perovskite structure with a tendency to retain rhombohedral structure even at higher PbTiO_3 content than that reported in bulk. We observe very large remnant polarization, ~75 microC/cm^2, and high dielectric constant, ~2400 at 1 kHz for x = 0.3, which lies in the MPB composition range. The unbuffered films show less than 1 microC/cm^2 for the same composition.

cond-mat.mtrl-sci↗

arXiv2008

Origin of high piezoelectric response of Pb(Zr_xTi_1-x)O_3 at the morphotropic phase boundary: Role of elastic instability

Temperature dependent structural changes in a nearly pure monoclinic phase composition (x=0.525) of Pb(Zr_xTi_1-x)O_3 (PZT) have been investigated using Rietveld analysis of high-resolution synchrotron powder x-ray diffraction data and correlated with changes in the dielectric constant and planar electromechanical coupling coefficient. Our results show that the intrinsic piezoelectric response of the tetragonal phase of PZT is higher than that of the monoclinic phase. It is also shown that the high piezoelectric response of PZT may be linked with an anomalous softening of the elastic modulus (1/S_11) of the tetragonal compositions closest to the morphotropic phase boundary.

cond-mat.mtrl-sci↗

arXiv2008

High-resolution synchrotron XRD study of Zr-rich compositions of Pb(Zr_xTi_1-x)O_3 (0.525\leq x \leq 0.60): evidence for the absence of the rhombohedral phase

Results of Rietveld analysis of the synchrotron XRD data on Pb(Zr_xTi_1-x)O_3 (PZT) for 0.525\leqx\leq0.60 are presented to show the absence of rhombohedral phase on the Zr-rich side of the morphotropic phase boundary (MPB). Our results reveal that the structure of PZT is monoclinic in the Cm space group for 0.525\leq x\leq 0.60. The nature of the monoclinic distortion changes from pseudo-tetragonal for 0.525\leqx\leq0.54 to pseudo-rhombohedral for x>0.54.

cond-mat.mtrl-sci↗

arXiv2007

A succession of relaxor ferroelectric transitions coexisting with ferroelectric states in Ba_0.55Sr_0.45TiO_3

We present here the results of frequency dependent dielectric, polarization and powder X-ray powder diffraction studies in the 300 to 100K temperature range for Ba_0.55Sr_0.45TiO_3. The dielectric results indicate a succession of three relaxor ferroelectric transitions accompanying the cubic to tetragonal to orthorhombic to rhombohedral phase transitions confirmed by XRD studies. Our results confirm the coexistence of the relaxor ferroelectric and ferroelectric behaviours.

cond-mat.mtrl-sci↗

arXiv2007

Soft Modes at the Stacking Faults in SiC Crystals

We use first-principles calculations based on density functional theory to determine and understand the driving force of the observed stacking fault expansion in SiC. We verify the suggestion based on recent experiments that the free energy difference between the faulted and the perfect structures is responsible for this expansion, and show that its origin lies in a large entropy associated with soft vibrational modes of the faulted SiC structure. These soft modes involve shearing of SiC on a long length-scale and are absent in related group IV semiconductors, such as Si, Ge and C.

cond-mat.mtrl-sci↗

arXiv2007

Dielectric Relaxation and Phase Transition at Cryogenic Temperatures in 0.65[Pb(Ni_1/3Nb_2/3)O_3]-0.35PbTiO_3 Ceramics

Dielectric measurements on 0.65[Pb(Ni_1/3Nb_2/3)O_3]-0.35PbTiO_3 ceramic in the temperature range 90K to 470K shows a relaxor ferroelectric transition around 350K with a Vogel-Fulcher freezing temperature of 338K and appearance of a non-ergodic relaxor ferroelectric phase of tetragonal structure at room temperature. This non-ergodic phase reenters into the relaxor state at low temperatures as evidenced by the appearance of a frequency dependent anomaly in the imaginary part of the dielectric constant around 160K, similar to those reported in other relaxor ferroelectric based morphotropic phase boundary ceramics. The polarization relaxation time for the 160K anomaly also follows Vogel-Fulcher type temperature dependence. Temperature dependent magnetization measurements show that this low temperature anomaly is not linked with any magnetic transition. Elastic modulus and low temperature x-ray diffraction (XRD) measurements reveal a tetragonal to monoclinic phase transition around 225K. It is argued that the low temperature dielectric dispersion around 160K results from the freezing of mesoscopic conformally miniaturized monoclinic domains formed inside the parent tetragonal domains below the structural phase transition temperature of 225K.

cond-mat.mtrl-sci↗

arXiv2007

Evidence for monoclinic crystal structure and negative thermal expansion below magnetic transition temperature in Pb(Fe_1/2Nb_1/2)O_3

The existing controversy about the room temperature structure of multiferroic Pb(Fe_1/2Nb_1/2)O_3 is settled using synchrotron powder x-ray diffraction data. Results of Rietveld refinements in the temperature range 300 to 12K reveal that the structure remains monoclinic in the Cm space group down to 12K, but the lattice parameters show anomalies at the magnetic transition temperature (T_N) due to spin lattice coupling. The lattice volume exhibits negative thermal expansion behaviour, with Alpha = - 4.64 x 10^-6 K^-1, below T_N.

cond-mat.mtrl-sci↗

arXiv2004

Barrier layer formation and PTCR effect in (1-x) Pb(Fe1/2Nb1/2)O3]-xPbTiO3 (x = 0.13) ceramics

(1-x)Pb(Fe1/2Nb1/2)O3-PbTiO3(PFN-xPT)Ceramics with x = 0.13 sintered at 1473K show diffuse phase transition and very high dielectric constant at lower frequencies.The high value of dielectric constant at lower frequencies is shown to be due to the barrier layer formation.The resistivity of the PFN-xPT ceramics, obtained by complex impedance analysis, initially decreases with temperature and then shows an upward trend beyond the ferroelectric Curie point reminiscent of BaTiO3 based thermistors with PTCR effect.

cond-mat.mtrl-sci↗