Linear–quadratic order parameter coupling and multiferroic phase transitions

The coupling between order parameters in systems with several instabilities has been analysed within Landau theory. The dominant term considered in this paper is linear in one order parameter and quadratic in the second order parameter ~QP2; other coupling terms have been treated previously. Typical examples for Q are proper or pseudo-proper ferroelastic instabilities, while P might be octahedral tilting in a perovskite, (anti-)ferromagnetic ordering or (anti-)ferroelectric soft modes. Coupling of this type is common in fluorites, Verwey transitions, Jahn-Teller systems, pnictide superconductors, etc. Analytical solutions and characteristic phase diagrams of the stable configurations are compiled. The coupling can lead to stepwise phase transitions even when the uncoupled systems would show continuous transitions. Mixed phases are common, so that many 'intermediate phases' described in the literature may be the result of this linear-quadratic coupling.     

Dynamics of cooperative Jahn-TellerT-systems

We consider a cubic crystal with a triply degenerate electronic ground-state in each unit cell (T-state). A linear Jahn-Teller interaction with acoustic phonons is assumed (T-e coupling). Below a critical temperatureT _c a tetragonal cooperative ordering is established. If a static crystal field splits the electronic states, an anticrossing of the cooperative excitation branches and the phonons in the smallk-regime is found. The resulting mixed modes are calculated (RPA and isotropic Debye model). The dispersion curves are given for specifick-directions and the temperature dependence is discussed.Supported by a grant from the Deutsche Forschungsgemeinschaft     

Synthesis and magnetic properties of CeVO3 nanostructures

CeVO₃ nanocrystals were fabricated by sintering CeVO₄ precursors in flowing hydrogen. Under an applied field of 20 Oe, a G-type orbital ordering transition, corresponding to the cooperative Jahn-Teller distortion, was enhanced and observed from the magnetization curve of CeVO₃ nanorods, different from that of the nanocrystallites. This enhancement of the orbital ordering transition depended on the giant magnetocrystalline anisotropy induced by strong crystallographic anisotropy. Furthermore, a stronger applied field decreased the anisotropy of electronic state induced by spatial shapes of orbitals and confined the cooperative Jahn-Teller distortion by lifting the orbital degeneracy, leading to the suppression of the orbital ordering transition.     

Influence of the Jahn-Teller effect on the structural, magnetic, and electrical properties of lightly doped manganites

Features of the structural, magnetic and electric properties in lightly doped La_1?x Sr _x MnO₃ (0.12 < x < 0.18) manganites are studied. Agreement between the types of orbital ordering and the local cooperative Jahn-Teller distortion octahedra is established. The interaction between the Jahn-Teller effect and magnetic ordering is described.     

Elastic properties of magnetic materials

This review discusses the theoretical aspects of magnetoelastic coupling with emphasis on the magnetic perturbation of elastic properties. The basic theory of magnetostriction is set out with application to ferromagnets, ferrimagnets and antiferromagnets, and is followed by a discussion of the physical origin of the magnetoelastic coupling coefficients in both localized and itinerant magnetic systems. Magnetic contributions to elastic compliance are then discussed and sound velocity anomalies near magnetic phase transitions investigated, including the cooperative Jahn-Teller limit for which the acoustic mode itself drives a structural transition even when magnetic ordering does not occur. The review concludes with discussion of magnetoelastic (or mixed magnon-phonon) waves in low temperature magnetically ordered phases and with a study of local striction phenomena in magnetically dilute materials. The latter leads to a recognition of internal rearrangement modes which may also be present in concentrated magnetic systems, and which may or may not couple significantly to bulk homogenous strain.     

La0.2Ca0.8MnO3材料电荷有序转变附近弹性模量的研究

通过超声与低频切变模量测量,得到多晶锰氧化物La0.2Ca0.8MnO3材料纵向模量与切变模量随温度变化关系曲线,发现在电荷有序转变温度附近,纵向模量与切变模量都出现最小值.运用合作Jahn-Teller效应理论对实验数据进行了拟合,发现理论与实验曲线符合较好,表明Jahn-Teller效应是发生电荷有序状态转变的主要机制之一.     

Transport in cooperativeT−(e+t) Jahn-Teller systems

A cooperative electron-phonon system is considered which exhibits a triply degenerate electronic ground state in each unit cell. As a model substance a simple cubic crystal is taken where each Jahn-Teller molecule has an octahedral surrounding. TheT electronic ground state is linearly coupled toe andt type vibrations with thee coupling dominating. By a unitary transformation the electron-phonon system is approximately decoupled. The remaining cooperative electron-electron system displays transport properties which are discussed in terms of a modified Maradudin formalism. Thermal conductivity is calculated by linear response theory. It is shown that in the transformed picture the phonon heat current approximately is independent from the pseudo spin heat current and the total thermal conductivity is given as a simple superposition of both contributions.Supported by a grant from the Deutsche Forschungsgemeinschaft     

Stabilization of A-type layered antiferromagnetic phase in LaMnO3 by cooperative Jahn-Teller deformations

It is shown that the layered antiferromagnetic order in stoechiometric cannot be understood purely from electronic interactions. On the contrary, it mainly results from strong cooperative Jahn-Teller deformation. Those involve a compression of the Mn-O octahedron along the c-axis (mode Q ₃ < 0), while alternate Jahn-Teller deformations occur in the ab-plane (mode Q₂). These deformations stabilize a certain type of orbital ordering. The resulting superexchange couplings are calculated by exact diagonalization, taking into account both e_g and t_2g orbitals. The main result is that antiferromagnetic (ferromagnetic) coupling along the c-direction (ab-planes) can be understood only if the Jahn-Teller energy is much larger than the superexchange couplings, which is consistent with experiments. This mechanism contrasts with that based on weak Jahn-Teller coupling which instead predicts elongation along the c-axis (Q ₃ > 0). The crucial role of the deformation anisotropy is also emphasized. Received 24 January 2000     

Influence of magnetic ordering on the structural properties of dilute copper ferrites

The x-ray structural properties of samples in the CuGa_xAl_xFe_2?2x O₄ (x = 0?0.7) and CuGa_xAl_2x Fe_2?3x O₄ (x = 0?0.5) systems are studied. It is found that magnetic ordering in dilute copper ferrites affects their structural properties. It is concluded that the frustration of magnetic coupling leads to suppression of the cooperative Jahn-Teller effect in dilute copper ferrites with a frustrated magnetic structure.     

XAFS investigation of the role of orientational disorder in the stabilization of the ferromagnetic metallic phase in nanoparticles of La(0.5)Ca(0.5)MnO3

The inclusion of the contribution of Jahn-Teller distortion of MnO(6) units, in addition to double-exchange, has been largely successful in explaining the magneto-transport behavior of manganites. However, our recent experiments on La(0.5)Ca(0.5)MnO(3) demonstrated the limitation of these factors in explaining the radical difference between the magneto-transport properties of bulk and nanocrystalline forms. While bulk La(0.5)Ca(0.5)MnO(3) exhibits insulator character (4-300 K) and an anti-ferromagnetic-ferromagnetic transition at 200 K, the nanocrystalline form stabilizes in a metallic ferromagnetic phase (4-300 K). This is counter-intuitive since large Jahn-Teller distortion, which promotes anti-ferromagnetism or insulator character, exists in the nanocrystals too (as indicated by x-ray diffraction results). In this work, we resolve this paradox by considering the role of structural disorder. Employing x-ray absorption spectroscopy, we establish that the disorder in inter-octahedral coupling is enhanced by 57% in the nanocrystals, as the octahedral units are randomly oriented with respect to each other. This orientational disorder promotes metallic ferromagnetism by destroying the stringent orbital ordering that is needed for anti-ferromagnetism and the co-operative nature of the orbital order.     

Origin of charge-orbital order in the half-doped manganites

The microscopic origin of the charge and orbital order in the half-doped manganites is examined from ab initio density-functional calculations and exact diagonalization studies. It is shown that the dominant mechanism responsible for the charge order is the Jahn-Teller coupling, with a lesser but significant contribution from the on-site Coulomb interaction. The band structure shows a sizable interchain coupling between the zigzag chains, leading to a considerable band dispersion normal to the chains, in sharp contrast with the zigzag chain physics.     

Temperature-dependent Brillouin scattering studies of surface acoustic modes in Nd0.5Sr0.5MnO3

Brillouin scattering experiments are carried out to study the surface acoustic waves in Nd_0.5Sr_0.5MnO₃ as a function of temperature in the range of 40-300 K covering the metal-insulator and charge-ordering phase transitions. The surface modes include surface Rayleigh wave, pseudo-surface acoustic wave (PSAW) and high velocity PSAW. The observed softening of the sound velocities for the surface modes below paramagnetic to ferromagnetic transition, T_c is related to the softening of the C₄₄ elastic constant. The subsequent hardening of the sound velocity below the charge ordering transition temperature T_co is attributed to the coupling of the acoustic phonon to the charge ordered state via long range ordering of the strong Jahn-Teller (JT) distortion.     

Direct observation of orbital ordering in La0.5Sr1.5MnO4 using soft x-ray diffraction

We report the first direct resonant soft x-ray scattering observations of orbital ordering. We have studied the low temperature phase of La0.5Sr1.5MnO4, a compound that displays charge and orbital ordering. Previous claims of orbital ordering in such materials have relied on observations at the manganese K edge. These claims have been questioned in several theoretical studies. Instead we have employed resonant soft x-ray scattering at the manganese L(III) and L(II) edges which probes the orbital ordering directly. Energy scans at constant wave vector are compared to theoretical predictions and suggest that at all temperatures there are two separate contributions to the scattering: direct orbital ordering and strong cooperative Jahn-Teller distortions of the Mn3+ ions.     

Roles of Electron Hopping on Orbital Ordering for Vanadium Spinels

We investigate the orbital ordering quantitatively for the spinel systems RV 2 O 4(R=Mg,Zn,Cd) in the viewpoint of single-ion physics through the method of diagonalization.Through the quantitative calculation,it is found that the spin-orbit(SO)coupling and the Jahn-Teller(JT) effect enable the orbital ordering under the conditions of negligible electron hopping among different V 3+ sites.For the systems RV 2 O 4,the electron hopping is implied to be observable from the energy gap in conductivity,so the orbital ordering of RV 2 O 4 cannot be induced by the SO coupling and JT effect at definite temperature,which is on contrary to the conclusions in [Phys.Rev.Lett.93(2004) 157206].     

Classical dimers and dimerized superstructure in an orbitally degenerate honeycomb antiferromagnet

We discuss the ground state of the spin-orbital model for spin-one ions with partially filled t_{2g} levels on a honeycomb lattice. We find that the orbital degrees of freedom induce a spontaneous dimerization of spins and drive them into nonmagnetic manifold spanned by hard-core dimer (spin-singlet) coverings of the lattice. The cooperative "dimer Jahn-Teller" effect is introduced through a magnetoelastic coupling and is shown to lift the orientational degeneracy of dimers leading to a peculiar valence bond crystal pattern. The present theory provides a theoretical explanation of nonmagnetic dimerized superstructure experimentally seen in Li2RuO3 compound at low temperatures.     

Polarization dependent chemistry of ferroelectric BaTiO3(001) domains

Recent works suggest that the surface chemistry, in particular the presence of oxygen vacancies, can affect the polarization in a ferroelectric material. This should, in turn, influence the domain ordering driven by the need to screen the depolarizing field. Here we show using density-functional theory that the presence of oxygen vacancies at the surface of BaTiO(3)(001) preferentially stabilizes an inward pointing, P-, polarization. Mirror electron microscopy measurements of the domain ordering confirm the theoretical results.     

Roles of Electron Hopping on Orbital Ordering for Vanadium Spinels

We investigate the orbital ordering quantitatively for the spinel systems RV₂O₄ (R=Mg, Zn, Cd) in the viewpoint of single-ion physics through the method of diagonalization. Through the quantitative calculation, it is found that the spin-orbit (SO)coupling and the Jahn-Teller (JT) effect enable the orbital ordering under the conditions of negligible electron hopping among different V³⁺ sites. For the systems RV₂O₄, the electron hopping is implied to be observable from the energy gap in conductivity, so the orbital ordering of RV₂O₄ cannot be induced by the SO coupling and JT effect at definite temperature, which is on contrary to the conclusions in [Phys. Rev. Lett. 93 (2004) 157206].     

Phase transitions in crystals with competitive Jahn-Teller subsystems

A statistical thermodynamic model of phase transformations caused by the cooperative Jahn-Teller effect in spinels containing two types of Jahn-Teller cations has been proposed. It has been shown that the specific features of the phase diagrams of compounds similar to Cu_{1 ? x} Ni _x Cr₂O₄, such as the presence of one orthorhombic and two anti-isostructural tetragonal phases, are associated with the competition between orderings of the subsystems of tetrahedra distorted due to the Jahn-Teller effect. The degree and character of the ordering of each subsystem of the solid solution have been determined. The main factors responsible for the thermodynamic properties and phase diagrams, in particular, the conditions for splitting of an isolated critical point into two triple points, have been investigated.     

Influence of the Jahn-Teller distortion on magnetic ordering in TbMn_1-xFe_xO₃

The Jahn-Teller distortion plays an important role in determining the exchange interaction in rare-earth manganites.In this work we study the influence of the Jahn-Teller distortion on the magnetic structures of TbMn1-xFexO3(x = 0,0.02,0.05,0.10,and 0.20) single crystals in the basal MnO2 plane.The decrease in the quadruple splitting with the increasing Fe doping indicates the reduction of the Jahn-Teller distortion,which makes the nearest neighboring(NN) FM interaction dominant over the next nearest neighbor(NNN) AFM interaction.This alteration is favorable for the development of A-type AFM ordering instead of the spiral magnetic ordering,which collapses when x ≥ 0.05.The analysis of dielectric data indicates that the ferroelectricity is arising from the peculiar spiral magnetic ordering.     

Does the self-trapped magnetic polaron exist in electron-doped manganites?

We show from ab initio density-functional calculations and model studies that, in the electron-doped manganite LaxCa1-xMnO3 (x<1), unbound electrons are introduced into the conduction band, which then trap themselves in the exchange-induced magnetic potential wells forming the self-trapped magnetic polarons (STMP). Hopping beyond the nearest neighbors drastically reduces the binding energy, while the Jahn-Teller coupling increases it somewhat, resulting in a net binding of about 100+/-20 meV. The electron is self-trapped in a seven-site ferromagnetic region, beyond which the lattice is essentially antiferromagnetic. In light of the recent experiments of Neumeier and Cohn, our results suggest that the STMP may be present in the lightly electron-doped manganites.