The carbon content of Earth and its core.

Earth's core is likely the largest reservoir of carbon (C) in the planet, but its C abundance has been poorly constrained because measurements of carbon's preference for core versus mantle materials at the pressures and temperatures of core formation are lacking. Using metal-silicate partitioning experiments in a laser-heated diamond anvil cell, we show that carbon becomes significantly less siderophile as pressures and temperatures increase to those expected in a deep magma ocean during formation of Earth's core. Based on a multistage model of core formation, the core likely contains a maximum of 0.09(4) to 0.20(10) wt% C, making carbon a negligible contributor to the core's composition and density. However, this accounts for ∼80 to 90% of Earth's overall carbon inventory, which totals 370(150) to 740(370) ppm. The bulk Earth's carbon/sulfur ratio is best explained by the delivery of most of Earth's volatiles from carbonaceous chondrite-like precursors.

A magma ocean origin to divergent redox evolutions of rocky planetary bodies and early atmospheres.

Magma oceans were once ubiquitous in the early solar system, setting up the initial conditions for different evolutionary paths of planetary bodies. In particular, the redox conditions of magma oceans may have profound influence on the redox state of subsequently formed mantles and the overlying atmospheres. The relevant redox buffering reactions, however, remain poorly constrained. Using first-principles simulations combined with thermodynamic modeling, we show that magma oceans of Earth, Mars, and the Moon are likely characterized with a vertical gradient in oxygen fugacity with deeper magma oceans invoking more oxidizing surface conditions. This redox zonation may be the major cause for the Earth's upper mantle being more oxidized than Mars' and the Moon's. These contrasting redox profiles also suggest that Earth's early atmosphere was dominated by CO2 and H2O, in contrast to those enriched in H2O and H2 for Mars, and H2 and CO for the Moon.

Evidence for Fe-Si-O liquid immiscibility at deep Earth pressures.

Seismic observations suggest that the uppermost region of Earth's liquid outer core is buoyant, with slower velocities than the bulk outer core. One possible mechanism for the formation of a stably stratified layer is immiscibility in molten iron alloy systems, which has yet to be demonstrated at core pressures. We find immiscibility between liquid Fe-Si and Fe-Si-O persisting to at least 140 GPa through a combination of laser-heated diamond-anvil cell experiments and first-principles molecular dynamics simulations. High-pressure immiscibility in the Fe-Si-O system may explain a stratified layer atop the outer core, complicate differentiation and evolution of the deep Earth, and affect the structure and intensity of Earth's magnetic field. Our results support silicon and oxygen as coexisting light elements in the core and suggest that [Formula: see text] does not crystallize out of molten Fe-Si-O at the core-mantle boundary.

Viscosity jump in the lower mantle inferred from melting curves of ferropericlase.

Convection provides the mechanism behind plate tectonics, which allows oceanic lithosphere to be subducted into the mantle as "slabs" and new rock to be generated by volcanism. Stagnation of subducting slabs and deflection of rising plumes in Earth's shallow lower mantle have been suggested to result from a viscosity increase at those depths. However, the mechanism for this increase remains elusive. Here, we examine the melting behavior in the MgO-FeO binary system at high pressures using the laser-heated diamond-anvil cell and show that the liquidus and solidus of (Mg x Fe1-x )O ferropericlase (x = ~0.52-0.98), exhibit a local maximum at ~40 GPa, likely caused by the spin transition of iron. We calculate the relative viscosity profiles of ferropericlase using homologous temperature scaling and find that viscosity increases 10-100 times from ~750 km to ~1000-1250 km, with a smaller decrease at deeper depths, pointing to a single mechanism for slab stagnation and plume deflection.

Using stepped anvils to make even insulation layers in laser-heated diamond-anvil cell samples.

We describe a method to make even insulation layers for high-pressure laser-heated diamond-anvil cell samples using stepped anvils. The method works for both single-sided and double-sided laser heating using solid or fluid insulation. The stepped anvils are used as matched pairs or paired with a flat culet anvil to make gasket insulation layers and not actually used at high pressures; thus, their longevity is ensured. We compare the radial temperature gradients and Soret diffusion of iron between self-insulating samples and samples produced with stepped anvils and find that less pronounced Soret diffusion occurs in samples with even insulation layers produced by stepped anvils.

Effect of laser annealing of pressure gradients in a diamond-anvil cell using common solid pressure media.

Pressure media are one of the most effective deterrents of pressure gradients in diamond-anvil cell (DAC) experiments. The media, however, become less effective with increasing pressure, particularly for solid pressure media. One of the most popular ways of alleviating the increase in pressure gradients in DAC samples is through laser annealing of the sample. We explore the effectiveness of this technique for six common solid pressure media that include: alkali metal halides LiF, NaCl, KCl, CsCl, KBr, as well as amorphous SiO2. Pressure gradients are determined through the analysis of the first-order diamond Raman band across the sample before and after annealing the sample with a near-infrared laser to temperatures between ~2000 and 3000 K. As expected, we find that in the absence of sample chamber geometrical changes and diamond anvil damage, laser annealing reduces pressure gradients, albeit to varying amounts. We find that under ideal conditions, NaCl provides the best deterrent to pressure gradients before and after laser annealing, at least up to pressures of 60 GPa and temperatures between ~2000 and 3000 K. Amorphous SiO2, on the other hand, transforms in to harder crystalline stishovite upon laser annealing at high pressures resulting in increased pressure gradients upon further compression without laser annealing.

Mapping temperatures and temperature gradients during flash heating in a diamond-anvil cell.

Here, we couple two-dimensional, 4-color multi-wavelength imaging radiometry with laser flash heating to determine temperature profiles and melting temperatures under high pressures in a diamond-anvil cell. This technique combines the attributes of flash heating (e.g., minimal chemical reactions, thermal runaway, and sample instability), with those of multi-wavelength imaging radiometry (e.g., 2D temperature mapping and reduction of chromatic aberrations). Using this new technique in conjunction with electron microscopy makes a powerful tool to determine melting temperatures at high pressures generated by a diamond-anvil cell.

Efficient graphite ring heater suitable for diamond-anvil cells to 1300 K.

In order to generate homogeneous high temperatures at high pressures, a ring-shaped graphite heater has been developed to resistively heat diamond-anvil cell (DAC) samples up to 1300 K. By putting the heater in direct contact with the diamond anvils, this graphite heater design features the following advantages: (1) efficient heating: sample can be heated to 1300 K while the DAC body temperature remains less than 800 K, eliminating the requirement of a special alloy for the DAC; (2) compact design: the sample can be analyzed with in situ measurements, e.g., x-ray, optical, and electrical probes are possible. In particular, the side access of the heater allows for radial x-ray diffraction (XRD) measurements in addition to traditional axial XRD.

Crystal structure of graphite under room-temperature compression and decompression.

Recently, sophisticated theoretical computational studies have proposed several new crystal structures of carbon (e.g., bct-C(4), H-, M-, R-, S-, W-, and Z-carbon). However, until now, there lacked experimental evidence to verify the predicted high-pressure structures for cold-compressed elemental carbon at least up to 50 GPa. Here we present direct experimental evidence that this enigmatic high-pressure structure is currently only consistent with M-carbon, one of the proposed carbon structures. Furthermore, we show that this phase transition is extremely sluggish, which led to the observed broad x-ray diffraction peaks in previous studies and hindered the proper identification of the post-graphite phase in cold-compressed carbon.

Slip systems in MgSiO3 post-perovskite: implications for D'' anisotropy.

Understanding deformation of mineral phases in the lowermost mantle is important for interpreting seismic anisotropy in Earth's interior. Recently, there has been considerable controversy regarding deformation-induced slip in MgSiO(3) post-perovskite. Here, we observe that (001) lattice planes are oriented at high angles to the compression direction immediately after transformation and before deformation. Upon compression from 148 gigapascals (GPa) to 185 GPa, this preferred orientation more than doubles in strength, implying slip on (001) lattice planes. This contrasts with a previous experiment that recorded preferred orientation likely generated during the phase transformation rather than deformation. If we use our results to model deformation and anisotropy development in the D'' region of the lower mantle, shear-wave splitting (characterized by fast horizontally polarized shear waves) is consistent with seismic observations.

Achieving high-density states through shock-wave loading of precompressed samples.

Materials can be experimentally characterized to terapascal pressures by sending a laser-induced shock wave through a sample that is precompressed inside a diamond-anvil cell. This combination of static and dynamic compression methods has been experimentally demonstrated and ultimately provides access to the 10- to 100-TPa (0.1-1 Gbar) pressure range that is relevant to planetary science, testing first-principles theories of condensed matter, and experimentally studying a new regime of chemical bonding.

Laser-driven shock experiments on precompressed water: Implications for "icy" giant planets.

Laser-driven shock compression of samples precompressed to 1 GPa produces high-pressure-temperature conditions inducing two significant changes in the optical properties of water: the onset of opacity followed by enhanced reflectivity in the initially transparent water. The onset of reflectivity at infrared wavelengths can be interpreted as a semiconductor<-->electronic conductor transition in water, and is found at pressures above approximately 130 GPa for single-shocked samples precompressed to 1 GPa. Our results indicate that conductivity in the deep interior of "icy" giant planets is greater than realized previously because of an additional contribution from electrons.