arXiv subjects

Yansun Yao

Publications and source records attributed to Yansun Yao.

13 recordsLinked to original sources

arXiv2025

On the ambient conditions crystal structure of AgSbTe2

We present a combined X-ray and neutron diffraction, Raman spectroscopy, and 121Sb NMR studies of AgSbTe2, supported by first-principles calculations aiming to elucidate its crystal structure. While diffraction methods cannot unambiguously resolve the structure, Raman and NMR data, together with electric field gradient calculations, strongly support the rhombohedral R-3m phase. Moreover, the agreement between experimental and calculated Raman spectra further corroborates this result, resolving the 60-year sold debate about the exact crystal structure of the AgSbTe2 compound.

cond-mat.mtrl-sci↗

arXiv2025

Emergence of Diffusional Hydrogen Escape in High-$T_c$ Superconducting Calcium Superhydride at Megabar Pressures

High-pressure metal superhydrides have attracted intense scientific interest due to their remarkable superconducting properties. While superconductivity is known to be sensitive to material composition, compositional variability is often overlooked in metal superhydrides at megabar pressures. Using ab initio path-integral simulations, we find that up to 7 % of the hydrogen atoms escape from the 215-kelvin superconducting CaH$_6$ upon decompression from 165 to 123 GPa. This loss of hydrogen leads to an elastic instability at low pressures, an "abnormal" positive pressure dependence of the superconducting $T_c$ and a quantum phase transition from a mixed superconducting-diffusive state to a pure superconducting phase. In this mixed phase, proton diffusivity reaches $10^{-8}$ $\mathrm{cm^2/s}$ at low temperatures and promotes to $10^{-7}$ $\mathrm{cm^2/s}$ at room temperature, which elucidates the escape of hydrogen at megabar pressures. Our results are consistent with many "anomalous" experimental observations and highlight the significance of composition effects in high-$T_c$ metal superhydrides.

cond-mat.supr-con↗

arXiv2024

The Critical Metallization of Hydrogen in Pressurized LaBeH8 Hydride

Behaviours of hydrogen, such as fluidity and metallicity, are crucial for our understanding of planetary interiors and the emerging field of high-temperature superconducting hydrides. These behaviours were discovered in complex phase diagrams of hydrogen and hydrides, however, the transition mechanism of behaviours driven by temperature, pressure and chemical compression remain unclear, particularly in the processes of metallization. Until now, a comprehensive theoretical framework to quantify atomization and metallization of hydrogen in phase diagram of hydrides has been lacking. In this study, we address this gap by combining molecular dynamics and electronic structure analysis to propose a theoretical framework, which clarify the content and properties of atomic hydrogen under various temperature and pressure conditions and chemical compression exerted by non-hydrogen elements in hydrides. Applying this framework to the superconducting hydride LaBeH8, we identify three general hydrogen orderings within its phase diagram: molecular, sublattice and warm hydrogens. During the phase transition from molecule to sublattice, hydrogen exhibits different properties from three general hydrogen orderings, such as fast superionicity, metallicity and unusual atomic content response to temperature. These abnormal behaviours were defined as the critical metallization of hydrogen, which not only suggests a potential synthesis route for the metastable phase but also provides valuable insights into the complex synthetic products of superconducting hydrides.

cond-mat.mtrl-sci↗

arXiv2024

Theoretical evidence of H-He demixing under Jupiter and Saturn conditions

The immiscibility of hydrogen-helium mixture under the temperature and pressure conditions of planetary interiors is crucial for understanding the structures of gas giant planets (e.g., Jupiter and Saturn). While the experimental probe at such extreme conditions is challenging, theoretical simulation is heavily relied in an effort to unravel the mixing behavior of hydrogen and helium. Here we develop a method via a machine learning accelerated molecular dynamics simulation to quantify the physical separation of hydrogen and helium under the conditions of planetary interiors. The immiscibility line achieved with the developed method yields substantially higher demixing temperatures at pressure above 1.5 Mbar than earlier theoretical data, but matches better to the experimental estimate. Our results suggest a possibility that H-He demixing takes place in a large fraction of the interior radii of Jupiter and Saturn, i.e., 27.5% in Jupiter and 48.3% in Saturn. This indication of an H-He immiscible layer hints at the formation of helium rain and offers a potential explanation for the decrease of helium in the atmospheres of Jupiter and Saturn.

physics.comp-ph↗

arXiv2024

Prediction of Room-Temperature Superconductivity in Quasi-atomic H2-Type Hydrides at High Pressure

Achieving superconductivity at room temperature (RT) is a holy grail in physics. Recent discoveries on high-Tc superconductivity in binary hydrides H3S and LaH10 at high pressure have directed the search for RT superconductors to compress hydrides with conventional electron-phonon mechanisms. Here, we predict an exceptional family of superhydrides under high pressures, MH12 (M = Mg, Sc, Zr, Hf, Lu), all exhibiting RT superconductivity with calculated Tcs ranging from 313 to 398 K. In contrast to H3S and LaH10, the hydrogen sublattice in MH12 is arranged as quasi-atomic H2 units. This unique configuration is closely associated with high Tc, attributed to the high electronic density of states derived from H2 antibonding states at the Fermi level and the strong electron-phonon coupling related to the bending vibration of H2 and H-M-H. Notably, MgH12 and ScH12 remain dynamically stable even at pressure below 100 GPa. Our findings offer crucial insights into achieving RT superconductivity and pave the way for innovative directions in experimental research.

cond-mat.supr-con↗

arXiv2023

Superconductivity in Li8Au electride

Located at crystal voids, interstitial anion electrons (IAEs) have diverse topologies, which may be tuned to achieve new properties. Elucidating the role of IAEs in electron-phonon coupling (EPC), and using it to design new electride superconductors, leads to the current prediction of superconducting Li8Au at high pressure. We suggest that the occurence of high-temperature superconductivity in electrides requires high-symmetry structures with hydrogen-like cages, an electron acceptor element to balance charges, and isolated IAEs coupled with medium-frequency vibrations. The uniquely designed Li8Au electride has a NaCl-type (B1) lattice, with atomic Au and cubic Li8 cages as bases. Isolated IAEs are formed at the cage centers, with extra charges taken up by Au. These octahedrally coordinated IAEs have a p-orbital-like attribute and are strongly coupled with atomic vibrations in the Li8 cages. The strong EPC in Li8Au results in a calculated Tc of 73.1 K at 250 GPa, which is the highest Tc reported to date for all the electrides. A slight substitutional Pt doping can enhance the Tc of Li8Au to exceed liquid nitrogen temperature.

cond-mat.supr-con↗

arXiv2023

Pressure-Induced Superconductivity in Topological Heterostructure (PbSe)5(Bi2Se3)6

Recently, the natural heterostructure of (PbSe)5(Bi2Se3)6 has been theoretically predicted and experimentally confirmed as a topological insulator. In this work, we induce superconductivity in (PbSe)5(Bi2Se3)6 by implementing high pressure. As increasing pressure up to 10 GPa, superconductivity with Tc ~ 4.6 K suddenly appears, followed by an abrupt decrease. Remarkably, upon further compression above 30 GPa, a new superconducting state arises, where pressure raises the Tc to an unsaturated 6.0 K within the limit of our research. Combining XRD and Raman spectroscopies, we suggest that the emergence of two distinct superconducting states occurs concurrently with the pressure-induced structural transition in this topological heterostructure (PbSe)5(Bi2Se3)6.

cond-mat.supr-con↗

arXiv2022

Size-Dependent Nucleation in Crystal Phase Transition from Machine Learning Metadynamics

In this work, we present an efficient framework that combines machine learning potential (MLP) and metadynamics to explore multi-dimensional free energy surfaces for investigating solid-solid phase transition. Based on the spectral descriptors and neural networks regression, we have developed a computationally scalable MLP model to warrant an accurate interpolation of the energy surface where two phases coexist. Applying the framework to the metadynamics simulation of B4-B1 phase transition of GaN under 50 GPa with different model sizes, we observe the sequential change of phase transition mechanism from collective modes to nucleation and growths. When the system size is at or below 128 000 atoms, the nucleation and growth appear to follow a preferred direction. At larger sizes, the nucleation tends to occur at multiple sites simultaneously and grow to microstructures by passing the critical size. The observed change of atomistic mechanism manifests the importance of statistical sampling with large system size. The combination of MLP and metadynamics is likely to be applicable to a broad class of induced reconstructive phase transitions at extreme conditions.

cond-mat.mtrl-sci↗

arXiv2021

En route to high Tc superconductivity via Rb substitution of guest metal atoms in SrB3C3 clathrate

Recently, a host/guest clathrate SrB3C3 with sp3-bonded boron-carbon framework was synthesized at around 50 GPa. On the basis of electron count, the structure is understood as guest Sr2+ cations intercalated in the (B3C3)3- framework. Previous calculations suggest that SrB3C3 is a hole conductor with an estimated superconducting critical temperature (Tc) of 42 K at ambient pressure. If atoms with similar radius, such as Rb, can substitute Sr2+ in the lattice, the electronic as well as superconductivity properties of this material will be modified significantly. Here, we perform extensive simulations on the stability and physical properties of Rb-Sr-B3C3 system using first-principles density functional calculation in combination with cluster expansion and CALYPSO structure prediction method. We predict a phonon-mediated superconductor Rb0.5Sr0.5B3C3 with a remarkably high Tc of 78 K at ambient pressure, which is a significant improvement from the estimated value (42 K) in SrB3C3. The current results suggest that substitution of alkali atom in synthesized clathrate SrB3C3 is a viable route toward high-Tc compounds.

cond-mat.mtrl-sci↗

arXiv2021

Design Principles for High Temperature Superconductors with Hydrogen-based Alloy Backbone at Moderate Pressure

Hydrogen-based superconductors provide a route to the long-sought goal of room-temperature superconductivity, but the high pressures required to metallize these materials limit their immediate application. For example, carbonaceous sulfur hydride, the first room-temperature superconductor, can reach a critical temperature (Tc) of 288 K only at the extreme pressure of 267 GPa. The next recognized challenge is the realization of room-temperature superconductivity at significantly lower pressures. Here, we propose a strategy for the rational design of high-temperature superconductors at low pressures by alloying small-radius elements and hydrogen to form ternary hydride superconductors with alloy backbones. We identify a hitherto unknown fluorite-type backbone in compositions of the form AXH8, which exhibit high temperature superconductivity at moderate pressures. The Fm-3m phase of LaBeH8, with a fluorite-type H-Be alloy backbone, is predicted to be metastable and superconducting with a Tc ~ 191 K at 50 GPa; a substantially lower pressure than that required by the geometrically similar clathrate hydride LaH10 (170 GPa). Our approach paves the way for finding high-Tc ternary hydride superconductors at conditions close to ambient pressures.

cond-mat.supr-con↗

arXiv2020

High-pressure structural study of a-Mn: solving a three decades-old mystery

Manganese, in the a-Mn structure, has been studied using synchrotron powder x-ray diffraction in a diamond anvil cell up to 220 GPa at room temperature combined with density functional calculations (DFT). The experiment reveals an extended pressure stability of the a-Mn phase up to the highest pressure of this study, in contrast with previous experimental and theoretical studies. On the other hand, calculations reveal that the previously predicted hcp-Mn phase becomes lower in enthalpy than the a-Mn phase above 160 GPa. The apparent discrepancy is explained due to a substantial electron transfer between Mn ions, which stabilizes the a-Mn phase through the formation of ionic bonding between monatomic ions under pressure.

cond-mat.mtrl-sci↗

arXiv2020

Hydrogen "penta-graphene-like" structure stabilized by hafnium: a high-temperature conventional superconductor

The recent discovery of H3S and LaH10 superconductors with record high superconducting transition temperatures, Tc, at high pressure, has fueled the search for room-temperature superconductivity in the compressed superhydrides. Here we predict the existence of an unprecedented hexagonal HfH10, with an extraordinarily high Tc of around 213-234 K at 250 GPa. In HfH10, the H atoms are arranged in clusters to form a planar "penta-graphene-like" sublattice, in contrast to the covalent sixfold cubic structure in H3S and clathrate-like structure in LaH10. The Hf atom acts as a "precompressor" and electron donor to the hydrogen sublattice. This "penta-graphene-like" H10 structure is also found in ZrH10, ScH10 and LuH10 at high pressure, each material showing a high Tc ranging from 134 to 220 kelvin. Our study of dense superhydrides with "penta-graphene-like" layered structures opens the door to the exploration and exploitation of a new class of high Tc superconductors.

cond-mat.supr-con↗

arXiv2017

Synthesis of Xenon and Iron/Nickel intermetallic compounds at Earth's core thermodynamic conditions

Although Xe is known to form stable compounds with strong electronegative elements, evidence on the formation of stable compounds with electropositive elements, such as Fe and Ni, was missing until very recently. In addition to the significance of the emerging field of noble gas elements chemistry, the possible formation of Xe-Fe/Ni compounds has been proposed as a plausible explanation of the so-called "missing Xe paradox". Here we explore the possible formation of stable compounds in the Xe-Fe/Ni systems at thermodynamic conditions representative of Earth's core. Using in situ synchrotron X-ray diffraction and Raman spectroscopy in concert with first principles calculations we demonstrate the synthesis of stable Xe(Fe,Fe/Ni)$_3$ and XeNi$_3$ compounds. The results indicate the changing chemical properties of elements under extreme conditions where noble gas elements can form stable compounds with elements which are electropositive at ambient conditions but become slightly electronegative at high pressures.

physics.chem-ph↗