264 research outputs found
Origin of the Verwey transition in magnetite: Group theory, electronic structure, and lattice dynamics study
The Verwey phase transition in magnetite has been analyzed using the group
theory methods. It is found that two order parameters with the symmetries
and induce the structural transformation from the high-temperature
cubic to the low-temperature monoclinic phase. The coupling between the order
parameters is described by the Landau free energy functional. The electronic
and crystal structure for the cubic and monoclinic phases were optimized using
the {\it ab initio} density functional method. The electronic structure
calculations were performed within the generalized gradient approximation
including the on-site interactions between 3d electrons at iron ions -- the
Coulomb element and Hund's exchange . Only when these local interactions
are taken into account, the phonon dispersion curves, obtained by the direct
method for the cubic phase, reproduce the experimental data. It is shown that
the interplay of local electron interations and the coupling to the lattice
drives the phonon order parameters and is responsible for the opening of the
gap at the Fermi energy. Thus, it is found that the metal-insulator transition
in magnetite is promoted by local electron interactions, which significantly
amplify the electron-phonon interaction and stabilize weak charge order
coexisting with orbital order of the occupied states at Fe ions. This
provides a scenario to understand the fundamental problem of the origin of the
Verwey transition in magnetite.Comment: 17 pages, 5 figures, 8 tables. Accepted version to be published in
Phys. Rev.
Magnetite: Raman study of the high-pressure and low-temperature effects
We report the results of a low-temperature (300K-15K) high-pressure (up to
22GPa) Raman study of the Verwey transition in magnetite (Fe3O4). We use
additional Raman modes observed below the Verwey transition to determine how
the transition temperature changes with the quasihydrostatic pressure. Increase
of the pressure results in the linear decrease of the Verwey transition
temperature, with no discontinuity. The corresponding pressure coefficient
dTV/dP is found to be ~ -5.2 K/GPa. Such a decrease is substantially larger
than the one predicted by the mean-field Coulomb interaction model of the
transition
Charge and orbital order in Fe_3O_4
Charge and orbital ordering in the low-temperature monoclinic structure of
magnetite (Fe_3O_4) is investigated using LSDA+U. While the difference between
t_{2g} minority occupancies of Fe^{2+}_B and Fe^{3+}_B cations is large and
gives direct evidence for charge ordering, the screening is so effective that
the total 3d charge disproportion is rather small. The charge order has a
pronounced [001] modulation, which is incompatible with the Anderson criterion.
The orbital order agrees with the Kugel-Khomskii theory.Comment: 4 pages, 2 figure
Spin-lattice instability to a fractional magnetization state in the spinel HgCr2O4
Magnetic systems are fertile ground for the emergence of exotic states when
the magnetic interactions cannot be satisfied simultaneously due to the
topology of the lattice - a situation known as geometrical frustration.
Spinels, AB2O4, can realize the most highly frustrated network of
corner-sharing tetrahedra. Several novel states have been discovered in
spinels, such as composite spin clusters and novel charge-ordered states. Here
we use neutron and synchrotron X-ray scattering to characterize the fractional
magnetization state of HgCr2O4 under an external magnetic field, H. When the
field is applied in its Neel ground state, a phase transition occurs at H ~ 10
Tesla at which each tetrahedron changes from a canted Neel state to a
fractional spin state with the total spin, Stet, of S/2 and the lattice
undergoes orthorhombic to cubic symmetry change. Our results provide the
microscopic one-to-one correspondence between the spin state and the lattice
distortion
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US-Japan Cooperative Program on neutron scattering
The US-Japan Cooperative Program on Neutron Scattering was implemented through arrangements by the United States Department of Energy with the Science and Technology Agency (STA) and the Ministry of Science, Education, and Culture (Monbusho) of Japan. It involves research collaboration in neutron scattering by Japanese scientists with scientists at Oak Ridge National Laboratory (ORNL) and Brookhaven National Laboratory (BNL) and the construction of new neutron scattering equipment at both laboratories with funds provided by the Japanese government. The United States provides neutrons in exchange for the new equipment, and other costs of the program are equally shared by the two countries. The assignments of Japanese scientists to ORNL and BNL vary in length, but they correspond to about two person years annually at each laboratory. An equal number of US scientists also participate in the research program. The main research collaboration is centered around the new equipment provided by the Japanese, but other facilities are utilized when they are needed. The new equipment includes a new type of wide-angle diffractometer and equipment for maintaining extreme sample environments at ORNL and a sophisticated polarized-beam triple-axis spectrometer at BNL. 13 refs., 3 figs
Complex-Orbital Order in Fe_3O_4 and Mechanism of the Verwey Transition
Electronic state and the Verwey transition in magnetite (Fe_3O_4) are studied
using a spinless three-band Hubbard model for 3d electrons on the B sites with
the Hartree-Fock approximation and the exact diagonalisation method.
Complex-orbital, e.g., 1/sqrt(2)[|zx> + i |yz>], ordered (COO) states having
noncollinear orbital moments ~ 0.4 mu_B on the B sites are obtained with the
cubic lattice structure of the high-temperature phase. The COO state is a novel
form of magnetic ordering within the orbital degree of freedom. It arises from
the formation of Hund's second rule states of spinless pseudo-d molecular
orbitals in the Fe_4 tetrahedral units of the B sites and ferromagnetic
alignment of their fictitious orbital moments. A COO state with longer
periodicity is obtained with pseudo-orthorhombic Pmca and Pmc2_1 structures for
the low-temperature phase. The state spontaneously lowers the crystal symmetry
to the monoclinic and explains experimentally observed rhombohedral cell
deformation and Jahn-Teller like distortion. From these findings, we consider
that at the Verwey transition temperature, the COO state remaining to be
short-range order impeded by dynamical lattice distortion in high temperature
is developed into that with long-range order coupled with the monoclinic
lattice distortion.Comment: 16 pages, 13 figures, 6 tables, accepted for publication in J. Phys.
Soc. Jp
Landau Model for Commensurate-Commensurate Phase Transitions in Uniaxial Improper Ferroelectric Crystals
We propose the Landau model for lock-in phase transitions in uniaxially
modulated improper ferroelectric incommensurate-commensurate systems of class
I. It includes Umklapp terms of third and fourth order and secondary order
parameter representing the local polarization. The corresponding phase diagram
has the structure of harmless staircase, with the allowed wave numbers obeying
the Farey tree algorithm. Among the stable commensurate phases only those with
periods equal to odd number of lattice constants have finite macroscopic
polarizations. These results are in excellent agreement with experimental
findings in some A2BX4 compounds.Comment: 9 pages, 5 figures, revtex, to be published in Journal of Physics:
Cond. Matter as a Letter to the Edito
Landau model for uniaxial systems with complex order parameter
We study the Landau model for uniaxial incommensurate-commensurate systems of
the I class by keeping Umklapp terms of third and fourth order in the expansion
of the free energy. It applies to systems in which the soft mode minimum lies
between the corresponding commensurate wave numbers. The minimization of the
Landau functional leads to the sine-Gordon equation with two nonlinear terms,
equivalent to the equation of motion for the well-known classical mechanical
problem of two mixing resonances. We calculate the average free energies for
periodic, quasiperiodic and chaotic solutions of this equation, and show that
in the regime of finite strengths of Umklapp terms only periodic solutions are
absolute minima of the free energy, so that the phase diagram contains only
commensurate configurations. The phase transitions between neighboring
configurations are of the first order, and the wave number of ordering goes
through harmless staircase with a finite number of steps. These results are the
basis for the interpretation of phase diagrams for some materials from the I
class of incommensurate-commensurate systems, in particular of those for
ABX and BCCD compounds. Also, we argue that chaotic barriers which
separate metastable periodic solutions represent an intrinsic mechanism for
observed memory effects and thermal hystereses.Comment: 12 pages, 14 figures, LaTeX, to be published in Phys. Rev.
Universal mechanism of discontinuity of commensurate-incommensurate transitions in three-dimensional solids: Strain dependence of soliton self-energy
We show that there exists a universal mechanism of long-range soliton
attraction in three-dimensional solids and, therefore, of discontinuity of any
commensurate-incommensurate (C-IC) phase transition. This mechanism is due to
the strain dependence of the soliton self-energy and specific features of the
solid-state elasticity. The role of this mechanism is studied in detail for a
class of C-IC transitions where the IC modulation is one-dimensional, the
anisotropy in the order parameter space is small, and the symmetry of the
systems allows the existence of the Lifshitz invariant. Two other mechanisms of
soliton attraction are operative here but the universal mechanism considered in
this paper is found to be the most important one in some cases. Comparison with
the most extensively studied C-IC transition in shows that the
experimentally observed thermal anomalies can be understood as a result of the
smearing of the theoretically predicted discontinuous transition.Comment: 8 pages (extended version, title changed
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