247 research outputs found
Structural investigations on -FeGe at high pressure and low temperature
The structural parameters of -FeGe have been determined at ambient
conditions using single crystal refinement. Powder diffraction have been
carried out to determine structural properties and compressibility for
pressures up to 30 GPa and temperatures as low as 82 K. The discontinuous
change in the pressure dependence of the shortest Fe-Ge interatomic distance
might be interpreted as a symmetry-conserving transition and seems to be
related to a magnetic phase boundary line.Comment: 4 pages, 5 figure
Quantum and Classical Orientational Ordering in Solid Hydrogen
We present a unified view of orientational ordering in phases I, II, and III
of solid hydrogen. Phases II and III are orientationally ordered, while the
ordering objects in phase II are angular momenta of rotating molecules, and in
phase III the molecules themselves. This concept provides quantitative
explanation of the vibron softening, libron and roton spectra, and increase of
the IR vibron oscillator strength in phase III. The temperature dependence of
the effective charge parallels the frequency shifts of the IR and Raman
vibrons. All three quantities are linear in the order parameter.Comment: Replaced with the final text, accepted for publication in PRL. 1 Fig.
added. Misc. text revision
Two pressure-induced structural phase transitions in TiOCl
We studied the crystal structure of TiOCl up to pressures of =25~GPa at
room temperature by x-ray powder diffraction measurements. Two pressure-induced
structural phase transitions are observed: At 15~GPa emerges
an 22 superstructure with -axis unique monoclinic
symmetry (space group P2/). At 22~GPa all lattice
parameters of the monoclinic phase show a pronounced anomaly. A fraction of the
sample persists in the ambient orthorhombic phase (space group ) over the
whole pressure range.Comment: 5 pages, 5 figures; accepted for publication in Phys. Rev.
Pressure-induced metallization and structural phase transition of the Mott-Hubbard insulator TiOBr
We investigated the pressure-dependent optical response of the
low-dimensional Mott-Hubbard insulator TiOBr by transmittance and reflectance
measurements in the infrared and visible frequency range. A suppression of the
transmittance above a critical pressure and a concomitant increase of the
reflectance are observed, suggesting a pressure-induced metallization of TiOBr.
The metallic phase of TiOBr at high pressure is confirmed by the presence of
additional excitations extending down to the far-infrared range. The
pressure-induced metallization coincides with a structural phase transition,
according to the results of x-ray powder diffraction experiments under
pressure.Comment: 4 pages, 3 figure
Transparent dense sodium
Under pressure, metals exhibit increasingly shorter interatomic distances.
Intuitively, this response is expected to be accompanied by an increase in the
widths of the valence and conduction bands and hence a more pronounced
free-electron-like behaviour. But at the densities that can now be achieved
experimentally, compression can be so substantial that core electrons overlap.
This effect dramatically alters electronic properties from those typically
associated with simple free-electron metals such as lithium and sodium, leading
in turn to structurally complex phases and superconductivity with a high
critical temperature. But the most intriguing prediction - that the seemingly
simple metals Li and Na will transform under pressure into insulating states,
owing to pairing of alkali atoms - has yet to be experimentally confirmed. Here
we report experimental observations of a pressure-induced transformation of Na
into an optically transparent phase at 200 GPa (corresponding to 5.0-fold
compression). Experimental and computational data identify the new phase as a
wide bandgap dielectric with a six-coordinated, highly distorted
double-hexagonal close-packed structure. We attribute the emergence of this
dense insulating state not to atom pairing, but to p-d hybridizations of
valence electrons and their repulsion by core electrons into the lattice
interstices. We expect that such insulating states may also form in other
elements and compounds when compression is sufficiently strong that atomic
cores start to overlap strongly.Comment: Published in Nature 458, 182-185 (2009
Polarization and Strong Infra-Red Activity in Compressed Solid Hydrogen
Under a pressure of ~150 GPa solid molecular hydrogen undergoes a phase
transition accompanied by a dramatic rise in infra-red absorption in the vibron
frequency range. We use the Berry's phase approach to calculate the electric
polarization in several candidate structures finding large, anisotropic dynamic
charges and strongly IR-active vibron modes. The polarization is shown to be
greatly affected by the overlap between the molecules in the crystal, so that
the commonly used Clausius-Mossotti description in terms of polarizable,
non-overlapping molecular charge densities is inadequate already at low
pressures and even more so for the compressed solid.Comment: To appear in Phys. Rev. Let
How chemistry controls electron localization in 3d1 perovskites: A Wannier-function study
In the series of 3d1 t2g perovskites, SrVO3--CaVO3--LaTiO3--YTiO3 the
transition-metal d electron becomes increasingly localized and undergoes a Mott
transition between CaVO3 and LaTiO3. By defining a low-energy Hubbard
Hamiltonian in the basis of Wannier functions for the t2g LDA band and solving
it in the single-site DMFT approximation, it was recently shown[1] that
simultaneously with the Mott transition there occurs a strong suppression of
orbital fluctuations due to splitting of the t2g levels. The present paper
reviews and expands this work, in particular in the direction of exposing the
underlying chemical mechanisms by means of ab initio LDA Wannier functions
generated with the NMTO method. The Wannier functions for the t2g band exhibit
covalency between the transition-metal t2g, the large cation-d, and the
oxygen-p states; this covalency, which increases along the series, turns out to
be responsible not only for the splittings of the t2g levels, but also for
non-cubic perturbations of the hopping integrals, both of which are decisive
for the Mott transition. We find good agreement with the optical and
photoemission spectra, with the crystal-field splittings and orbital
polarizations recently measured for the titanates, and with the metallization
volume for LaTiO3. The metallization volume for YTiO3 is predicted. Using
super-exchange theory, we reproduce the observed magnetic orders in LaTiO3 and
YTiO3, but the results are sensitive to detail, in particular for YTiO3 which,
without the Jahn-Teller distortion, would be AFM C- or A-type, rather than FM.
Finally, we show that it possible to unfold the orthorhombic t2g LDA
bandstructure to a pseudocubic zone. In this zone, the lowest band is separated
from the two others by a direct gap and has a width, W_I, which is
significantly smaller than that, W, of the entire t2g band. The progressive
GdFeO3-type distortion favours electron localization by decreasing W, by
increasing the splitting of the t2g levels and by decreasing W_I. Our
conclusions concerning the roles of GdFeO3-type and JT distortions agree with
those of Mochizuki and Imada [2].Comment: Published version, final. For high resolution figures see
http://www.fkf.mpg.de/andersen/docs/pub/abstract2004+/pavarini_02.pd
Origin of complex crystal structures of elements at pressure
We present a unifying theory for the observed complex structures of the
sp-bonded elements under pressure based on nearly free electron picture (NFE).
In the intermediate pressure regime the dominant contribution to crystal
structure arises from Fermi-surface Brillouin zone (FSBZ) interactions -
structures which allow this are favoured. This simple theory explains the
observed crystal structures, transport properties, the evolution of internal
and unit cell parameters with pressure. We illustrate it with experimental data
for these elements and ab initio calculation for Li.Comment: 4 pages 5 figure
Crystal structure of solid Oxygen at high pressure and low temperature
Results of X-ray diffraction experiments on solid oxygen at low temperature
and at pressures up to 10 GPa are presented.A careful sample preparation and
annealing around 240 K allowed to obtain very good diffraction patterns in the
orthorhombic delta-phase. This phase is stable at low temperature, in contrast
to some recent data [Y. Akahama et al., Phys. Rev. B64, 054105 (2001)], and
transforms with decreasing pressure into a monoclinic phase, which is
identified as the low pressure alpha-phase. The discontinuous change of the
lattice parameters, and the observed metastability of the alpha-phase
increasing pressure suggest that the transition is of the first order.Comment: 4 pages with three figure
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