239 research outputs found
First Principles Calculations of Shock Compressed Fluid Helium
The properties of hot dense helium at megabar pressures were studied with two
first-principles computer simulation techniques, path integral Monte Carlo and
density functional molecular dynamics. The simulations predicted that the
compressibility of helium is substantially increased by electronic excitations
that are present in the hot fluid at thermodynamic equilibrium. A maximum
compression ratio of 5.24(4)-fold the initial density was predicted for 360 GPa
and 150000 K. This result distinguishes helium from deuterium, for which
simulations predicted a maximum compression ratio of 4.3(1). Hugoniot curves
for statically precompressed samples are also discussed.Comment: Accepted to publication in Physical Review Letter
Equation of state of cubic boron nitride at high pressures and temperatures
We report accurate measurements of the equation of state (EOS) of cubic boron
nitride by x-ray diffraction up to 160 GPa at 295 K and 80 GPa in the range
500-900 K. Experiments were performed on single-crystals embedded in a
quasi-hydrostatic pressure medium (helium or neon). Comparison between the
present EOS data at 295 K and literature allows us to critically review the
recent calibrations of the ruby standard. The full P-V-T data set can be
represented by a Mie-Gr\"{u}neisen model, which enables us to extract all
relevant thermodynamic parameters: bulk modulus and its first
pressure-derivative, thermal expansion coefficient, thermal Gr\"{u}neisen
parameter and its volume dependence. This equation of state is used to
determine the isothermal Gr\"{u}neisen mode parameter of the Raman TO band. A
new formulation of the pressure scale based on this Raman mode, using
physically-constrained parameters, is deduced.Comment: 8 pages, 7 figure
The S(0) structure in highly compressed hydrogen and the orientational transition
A calculation of the rotational S(0) frequencies in high pressure solid
para-hydrogen is performed. Convergence of the perturbative series at high
density is demonstrated by the calculation of second and third order terms. The
results of the theory are compared with the available experimental data to
derive the density behaviour of structural parameters. In particular, a strong
increase of the value of the lattice constant ratio and of the
internuclear distance is determined. Also a decrease of the anisotropic
intermolecular potential is observed which is attributed to charge transfer
effects. The structural parameters determined at the phase transition may be
used to calculate quantum properties of the rotationally ordered phase.Comment: accepted Europhysics Letter
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
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
Solid molecular hydrogen: The Broken Symmetry Phase
By performing constant-pressure variable-cell ab initio molecular dynamics
simulations we find a quadrupolar orthorhombic structure, of symmetry,
for the broken symmetry phase (phase II) of solid H2 at T=0 and P =110 - 150
GPa. We present results for the equation of state, lattice parameters and
vibronic frequencies, in very good agreement with experimental observations.
Anharmonic quantum corrections to the vibrational frequencies are estimated
using available data on H2 and D2. We assign the observed modes to specific
symmetry representations.Comment: 5 pages (twocolumn), 4 Postscript figures. To appear in Phys. Rev.
Let
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Creating the Core Conditions of Extra-solar and Solar Giant Planets
Materials can be experimentally characterized at high pressures and densities by sending a laser-induced shock wave through a sample that is pre-compressed inside a diamond-anvil cell. This combination of static- and dynamic-compression methods has been experimentally demonstrated, and ultimately provides access to the 10-100 TPa (0.1-1 Gbar) pressure range that is relevant to planetary science. We report on dynamical measurements of the high pressure compressibility of helium, hydrogen and helium/hydrogen mixtures up to 230 GPa by combining laser shocks and static compression in diamond anvil cells. The initial density of samples in these precompressed targets has been varied by a factor of 3. The measurements on the principal He Hugoniot, i.e with the initial density of cryo-helium, is extended above 100 GPa and a maximum of compression ratio of greater than 5-fold of the initial density is observed. Also, a strong decrease in compressibility is observed by increasing the initial density. A similar data set has been produced for precompressed H{sub 2} and a mixture of He and H{sub 2}
Monte Carlo Analysis of a New Interatomic Potential for He
By means of a Quadratic Diffusion Monte Carlo method we have performed a
comparative analysis between the Aziz potential and a revised version of it.
The results demonstrate that the new potential produces a better description of
the equation of state for liquid He. In spite of the improvement in the
description of derivative magnitudes of the energy, as the pressure or the
compressibility, the energy per particle which comes from this new potential is
lower than the experimental one. The inclusion of three-body interactions,
which give a repulsive contribution to the potential energy, makes it feasible
that the calculated energy comes close to the experimental result.Comment: 36 pages, LaTex, 11 PostScript figures include
A quantum fluid of metallic hydrogen suggested by first-principles calculations
It is generally assumed that solid hydrogen will transform into a metallic
alkali-like crystal at sufficiently high pressure. However, some theoretical
models have also suggested that compressed hydrogen may form an unusual
two-component (protons and electrons) metallic fluid at low temperature, or
possibly even a zero-temperature liquid ground state. The existence of these
new states of matter is conditional on the presence of a maximum in the melting
temperature versus pressure curve (the 'melt line'). Previous measurements of
the hydrogen melt line up to pressures of 44 GPa have led to controversial
conclusions regarding the existence of this maximum. Here we report ab initio
calculations that establish the melt line up to 200 GPa. We predict that subtle
changes in the intermolecular interactions lead to a decline of the melt line
above 90 GPa. The implication is that as solid molecular hydrogen is
compressed, it transforms into a low-temperature quantum fluid before becoming
a monatomic crystal. The emerging low-temperature phase diagram of hydrogen and
its isotopes bears analogies with the familiar phases of 3He and 4He, the only
known zero-temperature liquids, but the long-range Coulombic interactions and
the large component mass ratio present in hydrogen would ensure dramatically
different propertiesComment: See related paper: cond-mat/041040
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