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NASA NTRS1986

High pressure cosmochemistry applied to major planetary interiors: Experimental studies

The overall goal of this project is to determine properties of the H-He-C-N-O system, as represented by small molecules composed of these elements, that are needed to constrain theoretical models of the interiors of the major planets. Much of our work now concerns the H2O-NH3 system. This project is the first major effort to measure phase equilibria in binary fluid-solid systems in diamond anvil cells. Vibrational spectroscopy, direct visual observations, and X-ray crystallography of materials confined in externally heated cells are our primary experimental probes. We also are collaborating with the shockwave physics group at Lawrence Livermore Laboratory in studies of the equation of state of a synthetic Uranus fluid and molecular composition of this and other H-C-N-O materials under planetary conditions.

Nicol, M. F.↗

NASA NTRS1986

The ammonia-water phase diagram and its implications for icy satellites

A Holzapfel-type diamond anvil cell is used to determine the NH3 - H2O phase diagram in the region from 0 to 33 mole percent NH3, 240 to 370 K, and 0 to 5 GPa. The following phases were identified: liquid; water ices Ih, III, V, VI, VII, and VIII; ammonia monohydrate, NH3.H2O; and ammonia dihydrate NH3.2H2O. Ammonia dihydrate becomes prominent at moderate pressures (less than 1 GPa), with planetologically significant implications, including the possibility of layering in Titan's magma ocean.

Johnson, M. L.↗

NASA NTRS1987

High pressure cosmochemistry of major planetary interiors: Laboratory studies of the water-rich region of the system ammonia-water

Several studies relative to high pressure cosmochemistry of major planetary interiors are summarized. The behavior of gas-ice mixtures at very high pressures, studies of the phase diagram of (NH3) sub x (H2O) sub 1-x at pressures to 5GPa and temperatures from 240 to 370 K, single crystal growth of ammonia dihydrate at room temperature in order to determine their structures by x-ray diffraction, spectroscopy of chemical reactions during shock compression in order to evaluate how the reactions affect the interpretation of equation of state data obtained by shock methods, and temperature and x-ray diffraction measurements made on resistively heated wire in diamond anvil cells in order to obtain phase and structural data relevant to the interiors of terrestrial planets are among the studies discussed.

Nicol, Malcolm↗

NASA NTRS1987

The ammonia-water phase diagram and its implications for icy satellites

Johnson, Mary L.↗

NASA NTRS1988

Crystal structure and density of helium to 232 kbar

The properties of helium and hydrogen at high pressure are topics of great interest to the understanding of planetary interiors. These materials constitute 95 percent of the entire solar system. A technique was presented for the measurement of X-ray diffraction from single-crystals of low-Z condenses gases in a diamond-anvil cell at high pressure. The first such single-crystal X-ray diffraction measurements on solid hydrogen to 26.5 GPa were presented. The application of this technique to the problem of the crystal structure, equation of state, and phase diagram of solid helium is reported. Crucial for X-ray diffraction studies of these materials is the use of a synchrotron radiation source which provides high brillance, narrow collimation of the incident and diffracted X-ray beams to reduce the background noise, and energy-dispersive diffraction techniques with polychromatic (white) radiation, which provides high detection efficiency.

Mao, H. K.↗

NASA NTRS1988

Phase relationships in Fe-Ni alloys at high pressures and temperatures

Diffusionless phase transformations in Fe-Ni alloys with up to 35 wt pct Ni were studied using resistance-heated diamond anvil cells and synchrotron radiation. At temperatures up to 600 C and pressures up to 25 GPa, Fe-35 percent Ni showed only the face-centered cubic (fcc) phase while Fe-25 percent Ni and Fe-10 percent Ni showed the body-centered cubic (bcc) and hexagonal close-packed (hcp) phases in addition to the fcc phase. The phase relationships of these solid phases are topologically similar to those of pure iron. The triple point becomes lower in temperature, and the slope (dT/dP) of the fcc/hcp boundary decreased as Ni-content increases in the alloys. From these results it is inferred that Fe-Ni alloys in the earth's inner core might exist as two phases, fcc and hcp. The existence of these two phases could have played an important role in the separation of the inner and outer core.

Huang, Eugene↗

NASA NTRS1988

Phase transition in solid molecular hydrogen at ultrahigh pressures

Solid normal hydrogen was compressed in a diamond-anvil cell to pressures above 200 GPa. Spontaneous Raman spectra demonstrate that the solid undergoes a structural phase transformation beginning at 145 GPa at 77 K, as evidenced by an abrupt discontinuity in the intramolecular vibron frequency as a function of pressure. The magnitude of the vibron-frequency shift and the pressure-temperature conditions of the phase transformation are consistent with its identification as the theoretically predicted pressure-induced orientational ordering of the molecular solid.

Hemley, R. J.↗

NASA NTRS1989

Optical evidence for the metallization of Xenon at 132(5) GPa

Xe has been compressed in a diamond-anvil cell to approximately 200 GPa. The metallization of Xe by band-gap closure was investigated by obtaining optical data in both the metallic and insulating states. In the metallic state, the pressure dependence of the plasma frequency was determined from absorption data fitted with a free-electron model. In the insulating state, the pressure dependence of the band gap was determined from absorption data fitted with an indirect-band-gap model. The optical data indicate that the insulator-to-metal transition in Xe occurs at 132(5) GPa.

Goettel, Kenneth A.↗

NASA NTRS1989

Phase diagram for ammonia-water mixtures at high pressures - Implications for icy satellites

The (NH3)x(H2O)1-x phase diagram for X from 0 to 0.50 has been reexamined at temperatures from 125 K to 400 K and at pressures from 6.0 GPa using diamond anvil cells, and the implications of the findings for icy satellites are addressed. Titan is likely to have a thicker NH3-H2O ocean than previously suspected, because the stability field of NH3-H2O is found to be smaller than previously supposed. The implications for methane and ammonia volcanism on Titan are briefly discussed. The experimentally observed reactivity between the liquid and iron may also have implications for planetary and satellite evolution.

Cynn, H. C.↗

NASA NTRS1989

New transformations between crystalline and amorphous ice

High-pressure optical and spectroscopic techniques were used to obtain directly the ice I(h) - hda-ice transformation in a diamond-anvil cell, and the stability of the amorphous form is examined as functions of pressure and temperature. It is demonstrated that hda-ice transforms abruptly at 4 GPa and 77 K to a crystalline phase close in structure to orientationally disordered ice-VII and to a more highly ordered, ice-VIII-like structure at higher temperatures. This is the first time that an amorphous solid is observed to convert to a crystalline solid at low temperatures by compression alone. Phase transitions of this type may be relevant on icy planetary satellites, and there may also be implications for the high-pressure behavior of silica.

Hemley, R. J.↗

NASA NTRS1989

Isotope effects in dense solid hydrogen - Phase transition in deuterium at 190 + or - 20 GPa

Raman measurements of solid normal deuterium compressed in a diamond-anvil cell indicate that the material undergoes a structural phase transformation at 190 + or - 20 GPa and 77 K. Spectroscopically, the transition appears analogous to that observed in hydrogen at 145 + or - 5 GPa. The large isotope effect on the transition pressure suggests there is a significant vibrational contribution to the relative stability of the solid phases of hydrogen at very high densities.

Hemley, R. J.↗

NASA NTRS1990

High-pressure phase transition and equation of state of CsI

Stuructural properties of CsI at high pressure have been investigated by the use of synchrotron X-ray-diffraction techniques with the diamond-anvil cell at 300 K. The results indicate that the material undergoes a continuous distortion from B2 to an hcp-like phase, which is stable to at least 302 GPa. The intermediate orthorhombic phase is geometrically different from previous assignments and about 10 percent denser. With the new structure, the p-V results of static pressure experiments, shock-wave studies, and theoretical calculations are now in good agreement.

Mao, H. K.↗

NASA NTRS1990

Laboratory studies of the electrical conductivity of silicate perovskites at high pressures and temperatures

The electrical conductivities of two silicate perovskites and a perovskite-magnesiowuestite assemblage, all having an atomic ratio of Mg to Fe equal to 0.88/0.12, have been measured with alternating current and direct current (dc) techniques at simultaneously high pressures and temperatures. Measurements up to pressures of 80 GPa and temperatures of 3500 K, using a laser-heated diamond anvil cell, demonstrate that the electrical conductivity of these materials remains below 10-3 S/m at lower mantle conditions. The activation energies for electrical conduction are between 0.1 and 0.4 eV from the data, and the conduction in these perovskites is ascribed to an extrinsic electronic process. The new measurements are in agreement with a bound that was previously obtained from dc measurements for the high-PT conductivity of perovskite-dominated assemblages. The results show that the electrical conductivity of (Mg/0.88/Fe/0.12)SiO3 perovskite differs significantly from that of the earth's deep mantle, as inferred from geophysical observations.

Li, Xiaoyuan↗

NASA NTRS1990

High pressure-temperature electrical conductivity of magnesiowustite as a function of iron oxide concentration

The electrical conductivity of (Mg, Fe)O magnesiowustite containing 9 and 27.5 mol pct FeO has been measured at simultaneously high pressures (30-32 GPa) and temperatures using a diamond anvil cell heated with a continuous wave Nd:YAG laser and an external resistance heater. The conductivity depends strongly on the FeO concentration at both ambient and high pressures. At the pressures and temperatures of about 30 GPa and 2000 K, conditions expected in the lower mantle, the magnesiowustite containing 27.5 percent FeO is 3 orders of magnitude more conductive than that containing 9 percent FeO. The activation energy of magnesiowustite decreases with increasing iron concentration from 0.38 (+ or - 0.09) eV at 9 percent FeO to 0.29 (+ or - 0.05) eV at 27.5 percent FeO.

Li, Xiaoyuan↗

NASA NTRS1991

Ammonia-water mixtures at high pressures - Melting curves of ammonia dihydrate and ammonia monohydrate and a revised high-pressure phase diagram for the water-rich region

The phase relations of some mixtures of ammonia and water are investigated to create a phase diagram in pressure-temperature-composition space relevant to the geophysical study of bodies in the outer solar system. The mixtures of NH3(x)H2O(1-x), where x is greater than 0.30 but less than 0.51, are examined at pressures and temperatures ranging from 0-6.5 GPa and 125-400 K, respectively. The ruby luminescence technique monitors the pressure and a diamond-anvil cell compresses the samples, and the phases are identified by means of normal- and polarized-light optical microscopy. The melting curve for NH3H2O(2) is described by the equation T = 176 + 60P - 8.5P squared for the ranges of 0.06-1.4 GPa and 179-243 K. The equation for NH3H2O is T = 194 + 37P - P squared, which represents a minor correction of a previous description by Johnson et al. (1985). Observed phase transitions are consistent with the high-pressure stability limit of NH3H2O(2), and the transition boundary is found to be linear.

Boone, S.↗

NASA NTRS1991

Carbonate stability in the earth's mantle - A vibrational spectroscopic study of aragonite and dolomite at high pressures and temperatures

The structural changes of aragonite and dolomite taking place at high pressures and temperatures were investigated by measuring the Raman spectra of these materials to pressures of 23 and 28 GPa (generated in a diamond anvil cell), respectively; in addition, the IR spectra of aragonite were measured to 40 GPa. The spectroscopic data demonstrated that, at 300 K, dolomite and aragonite samples were stable to pressures of 28 and 41 GPa, respectively. No phase transitions were observed following heating of aragonite and dolomite to temperatures of 2000 K and 800 K, respectively. The mode Grueneisen parameters indicate that the carbonate group in these two minerals is relatively insensitive to pressure, with the dominant compaction mechanism being the compression of the Ca and Mg polyhedra.

Kraft, Susan↗

NASA NTRS1992

Simultaneous high-P, high-T X ray diffraction study of beta-(Mg,Fe)2SiO4 to 26 GPa and 900 K

Attention is given to the lattice parameters of beta phase (Mg(0.84)Fe(0.16))2SiO4 determined by X-ray diffraction using synchrotron radiation under simultaneous high-pressure and high-temperature conditions. The experiments were conducted up to a pressure of 26 GPa and a temperature of 900 K. High pressures were generated in a Mao-Bell type diamond anvil cell using neon gas as a pressure medium. The sample was heated with an external Ni80Cr20 wire heater. Gold was used as an internal high-pressure calibrant at high temperature. The experimental data indicated the anisotropic behavior of the beta phase at high pressure and temperature, i.e., the c axis is about 35-percent more expansible and about 25-percent more compressible than the a and b axes. A value of 5.1 +/-0.8 was found for the Anderson-Grueneisen parameter. The derived thermodynamic parameters for the beta phase are summarized.

Fei, Yingwei↗

NASA NTRS1992

Electronic energy gap of molecular hydrogen from electrical conductivity measurements at high shock pressures

Electrical conductivities were measured for liquid D2 and H2 shock compressed to pressures of 10-20 GPa (100-200 kbar), molar volumes near 8 cu cm/mol, and calculated temperatures of 2900-4600 K. The semiconducting energy gap derived from the conductivities is 12 eV, in good agreement with recent quasi-particle calculations and with oscillator frequencies measured in diamond-anvil cells.

Nellis, W. J.↗