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Register a new userAntiferrodistortive phase transition in EuTiO3
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X-ray diffraction, dynamical mechanical analysis and infrared reflectivity studies revealed an antiferrodistortive phase transition in EuTiO3 ceramics. Near 300K the perovskite structure changes from cubic Pm-3m to tetragonal I4/mcm due to antiphase tilting of oxygen octahedra along the c axis (a0a0c- in Glazer notation). The phase transition is analogous to SrTiO3. However, some ceramics as well as single crystals of EuTiO3 show different infrared reflectivity spectra bringing evidence of a different crystal structure. In such samples electron diffraction revealed an incommensurate tetragonal structure with modulation wavevector q ~ 0.38 a*. Extra phonons in samples with modulated structure are activated in the IR spectra due to folding of the Brillouin zone. We propose that defects like Eu3+ and oxygen vacancies strongly influence the temperature of the phase transition to antiferrodistortive phase as well as the tendency to incommensurate modulation in EuTiO3.
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Microscopic structural instabilities of EuTiO3 single crystal were investigated by synchrotron x-ray diffraction. Antiferrodistortive (AFD) oxygen octahedral rotational order was observed alongside Ti derived antiferroelectric (AFE) distortions. The competition between the two instabilities is reconciled through a cooperatively modulated structure allowing both to coexist. The electric and magnetic field effect on the modulated AFD order shows that the origin of large magnetoelectric coupling is based upon the dynamic equilibrium between the AFD - antiferromagnetic interactions versus the electric polarization - ferromagnetic interactions.
Epitaxial La0.7Sr0.3MnO3 (LSMO) thin films, with different thickness ranging from 20 nm up to 330 nm, were deposited on (100)-oriented strontium titanate (STO) substrates by pulsed laser deposition, and their structure and morphology characterized at room temperature. Magnetic and electric transport properties of the as-processed thin films reveal an abnormal behavior in the temperature dependent magnetization M(T) below the antiferrodistortive STO phase transition (TSTO) and also an anomaly in the magnetoresistance and electrical resistivity close to the same temperature. Up to 100 nm LSMO thin films, an in-excess magnetization and pronounced changes in the coercivity are evidenced, achieved through the interface-mediated magnetoelastic coupling with antiferrodistortive domain wall movement occurring below TSTO. Contrarily, for thicker LSMO thin films, above 100 nm, an in-defect magnetization is observed. This reversed behavior can be understood within the emergence in the upper layer of the film, observed by high resolution transmission electron microscopy, of a branched structure needed to relax elastic energy stored in the film which leads to randomly oriented magnetic domain reconstructions. For enough high-applied magnetic fields, as thermodynamic equilibrium is reached, a fully suppression of the anomalous magnetization occurs, wherein the temperature dependence of the magnetization starts to follow the expected Brillouin behavior.
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.
The ultrafast dynamics of the octahedral rotation in Ca:SrTiO3 is studied by time resolved x-ray diffraction after photo excitation over the band gap. By monitoring the diffraction intensity of a superlattice reflection that is directly related to the structural order parameter of the soft-mode driven antiferrodistortive phase in Ca:SrTiO3, we observe a ultrafast relaxation on a 0.2 ps timescale of the rotation of the oxygen octahedron, which is found to be independent of the initial temperaure despite large changes in the corresponding soft-mode frequency. A further, much smaller reduction on a slower picosecond timescale is attributed to thermal effects. Time-dependent density-functional-theory calculations show that the fast response can be ascribed to an ultrafast displacive modification of the soft-mode potential towards the normal state, induced by holes created in the oxygen 2p states.
The multiferroic properties of EuTiO3 are greatly enhanced when a sample is strained, signifying that coupling between strain and structural, magnetic or ferroelectric order parameters is extremely important. Here resonant ultrasound spectroscopy has been used to investigate strain coupling effects, as well as possible additional phase transitions, through their influence on elastic and anelastic relaxations that occur as a function of temperature between 2 and 300 K and with applied magnetic field up to 14 T. Antiferromagnetic ordering is accompanied by acoustic loss and softening, and a weak magnetoelastic effect is also associated with the change in magnetization direction below ~2.8 K. Changes in loss due to the influence of magnetic field suggest the existence of magnetic defects which couple with strain and may play a role in pinning of ferroelastic twin walls.
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