arXiv subjects

Hanyu Liu

Publications and source records attributed to Hanyu Liu.

80 records · Page 5Linked to original sources

arXiv2013

Xenon Reacts with Iron at the Conditions of the Earth's Core

Studies of the Earth's atmosphere have shown that more than 90% of xenon (Xe) is depleted compared with its abundance in chondritic meteorites. This long-standing missing Xe paradox has become the subject of considerable interest and several models for a Xe reservoir have been proposed. Whether the missing Xe is hiding in the Earth's core has remained a long unanswered question. The key to address this issue lies in the reactivity of Xe with iron (Fe, the main constituent of the Earth's core), which has been denied by earlier studies. Here we report on the first evidence of the chemical reaction of Xe and Fe at the conditions of the Earth's core, predicted through first-principles calculations and unbiased structure searching techniques. We find that Xe and Fe form a stable, inter-metallic compound of XeFe3, adopting a Cu3Au-type face-centered cubic structure above 183 GPa and at 4470 K. As the result of a Xe -> Fe charge transfer, Xe loses its chemical inertness by opening up the filled 5p electron shell and functioning as a 5p-like element, whilst Fe is unusually negatively charged, acting as an oxidant rather than a reductant as usual. Our work establishes that the Earth's core is a natural reservoir for Xe storage, and possibly provides the key to unlocking the missing Xe paradox.

physics.geo-ph↗

arXiv2013

Anomalous melting behavior of solid hydrogen at high pressures

Hydrogen is the most abundant element in the universe, and its properties under conditions of high temperature and pressure are crucial to understand the interior of of large gaseous planets and other astrophysical bodies. At ultra high pressures solid hydrogen has been predicted to transform into a quantum fluid, because of its high zero point motion. Here we report first principles two phase coexistence and Z method determinations of the melting line of solid hydrogen in a pressure range spanning from 30 to 600 GPa. Our results suggest that the melting line of solid hydrogen, as derived from classical molecular dynamics simulations, reaches a minimum of 367 K at about 430 GPa, at higher pressures the melting line of the atomics Cs IV phase regain a positive slope. In view of the possible importance of quantum effects in hydrogen at such low temperatures, we also determined the melting temperature of the atomic CsIV phase at pressures of 400, 500, 600 GPa, employing Feynman path integral simulations. These result in a downward shift of the classical melting line by about 100 K, and hint at a possible secondary maximum in the melting line in the region between 500 and 600 GPa, testifying to the importance of quantum effects in this system. Combined, our results imply that the stability field of the zero temperature quantum liquid phase, if it exists at all, would only occur at higher pressures than previously thought.

cond-mat.mtrl-sci↗

arXiv2012

Proton Transfer in Phase IV of Solid Hydrogen and Deuterium

The recent discovery of phase IV of solid hydrogen and deuterium consisting of two alternate layers of graphenelike three-molecule rings and unbound H2 molecules have generated great interests. However, vibrational nature of phase IV remains poorly understood. Here, we report a peculiar proton transfer and a simultaneous rotation of three molecule rings in graphenelike layers predicted by ab initio variable cell molecular dynamics simulations for phase IV of solid hydrogen and deuterium at pressure ranges of from 250 to 350 GPa and temperature range of from 300 to 500 K. This proton transfer is intimately related to the particular elongation of molecules in graphenelike layers, and it becomes more pronounced with increasing pressure at the course of larger elongation of molecules. As the consequence of proton transfer, hydrogen molecules in graphenelike layers are short lived and hydrogen vibration is strongly anharmonic. Our findings provide direct explanations on the observed abrupt increase of Raman width at the formation of phase IV and its large increase with pressure.

cond-mat.mtrl-sci↗

arXiv2012

Hybrid Functional Study Rationalizes the Simple Cubic Phase of Calcium at High Pressures

Simple cubic (SC) phase has been long experimentally determined as the high-pressure phase III of elemental calcium (Ca) since 1984. However, recent density functional calculations within semi-local approximation showed that this SC phase is structurally unstable by exhibiting severely imaginary phonons, and is energetically unstable with respect to a theoretical body-centered tetragonal I41/amd structure over the pressure range of phase III. These calculations generated extensive debates on the validity of SC phase. Here we have re-examined the SC structure by performing more precise density functional calculations within hybrid functionals of Heyd-Scuseria-Erhzerhof (HSE) and PBE0. Our calculations were able to rationalize fundamentally the phase stability of SC structure over all other known phases by evidence of its actual energetic stability above 33 GPa and its intrinsically dynamical stability without showing any imaginary phonons in the entire pressure range studied. We further established that the long-thought theoretical I41/amd structure remains stable in a narrow pressure range before entering SC phase and is actually the structure of experimental Ca-III' synthesized recently at low temperature 14 K as supported by the excellent agreement between our simulated X-ray diffraction patterns and the experimental data. Our results shed strong light on the crucial role played by the precise electron exchange energy in a proper description of the potential energy of Ca.

cond-mat.mtrl-sci↗

arXiv2012

Room-Temperature Structures of Solid Hydrogen at High Pressures

By employing first-principles metadynamics simulations, we explore the 300 K structures of solid hydrogen over the pressure range 150-300 GPa. At 200 GPa, we find the ambient-pressure disordered hexagonal close-packed (hcp) phase transited into an insulating partially ordered hcp phase (po-hcp), a mixture of ordered graphene-like H2 layers and the other layers of weakly coupled, disordered H2 molecules. Within this phase, hydrogen remains in paired states with creation of shorter intra-molecular bonds, which are responsible for the very high experimental Raman peak above 4000 cm-1. At 275 GPa, our simulations predicted a transformation from po-hcp into the ordered molecular metallic Cmca phase (4 molecules/cell) that was previously proposed to be stable only above 400 GPa. Gibbs free energy calculations at 300 K confirmed the energetic stabilities of the po-hcp and metallic Cmca phases over all known structures at 220-242 GPa and >242 GPa, respectively. Our simulations highlighted the major role played by temperature in tuning the phase stabilities and provided theoretical support for claimed metallization of solid hydrogen below 300 GPa at 300 K.

cond-mat.mtrl-sci↗

arXiv2012

Quasi-molecular and atomic phases of dense solid hydrogen

The high-pressure phases of solid hydrogen are of fundamental interest and relevant to the interior of giant planets; however, knowledge of these phases is far from complete. Particle swarm optimization (PSO) techniques were applied to a structural search, yielding hitherto unexpected high-pressure phases of solid hydrogen at pressures up to 5 TPa. An exotic quasi-molecular mC24 structure (space group C2/c, stable at 0.47-0.59 TPa) with two types of intramolecular bonds was predicted, providing a deeper understanding of molecular dissociation in solid hydrogen, which has been a mystery for decades. We further predicted the existence of two atomic phases: (i) the oC12 structure (space group Cmcm, stable at > 2.1 TPa), consisting of planar H3 clusters, and (ii) the cI16 structure, previously observed in lithium and sodium, stable above 3.5 TPa upon consideration of the zero-point energy. This work clearly revised the known zero-temperature and high-pressure (>0.47 TPa) phase diagram for solid hydrogen and has implications for the constituent structures of giant planets.

cond-mat.mtrl-sci↗

arXiv2011

Predicting Two-Dimensional Boron-Carbon Compounds by the Global Optimization Method

We adopt a global optimization method to predict two-dimensional (2D) nanostructures through the particle-swarm optimization (PSO) algorithm. By performing PSO simulations, we predict new stable structures of 2D boron-carbon (B-C) compounds for a wide range of boron concentrations. Our calculations show that: (1) All 2D B-C compounds are metallic except for BC3 which is a magic case where the isolation of carbon six-membered ring by boron atoms results in a semiconducting behavior. (2) For C-rich B-C compounds, the most stable 2D structures can be viewed as boron doped graphene structures, where boron atoms typically form 1D zigzag chains except for BC3 in which boron atoms are uniformly distributed. (3) The most stable 2D structure of BC has alternative carbon and boron ribbons with strong in-between B-C bonds, which possesses a high thermal stability above 2000K. (4) For B-rich 2D B-C compounds, there is a novel planar-tetracoordinate carbon motif with an approximate C2v symmetry.

cond-mat.mtrl-sci↗

arXiv2010

Anomalous optical and electronic properties of dense sodium

Based on ab initio density-functional-theory using generalized gradient approximation, we systematically study the optical and electronic properties of the insulating dense sodium phase (Na-hp4) reported recently [Ma \textit{et al.}, Nature \textbf{458}, 182 (2009)]. The structure is found optically anisotropic and transparent to visible light, which can be well interpreted using its electronic band structure and angular moment decomposed density of states. Through the bader analysis of Na-hp4 at different pressures, we conclude that ionicity exists in the structure and becomes stronger with increasing pressure. In addition, the absorption spectra in the energy range from 1.4 to 2.4 eV are compared with recent experimental results and found good agreement. It is found that the deep-lying valence electrons participate in the interband transition.

cond-mat.mtrl-sci↗