arXiv subjects

Stella Chariton

Publications and source records attributed to Stella Chariton.

At least 19 recordsLinked to original sources

arXiv2026

Two New Molecular Nitrogen Phases near Megabar Pressures

Molecular nitrogen exhibits remarkable structural diversity near the polymeric transition, where multiple phases are metastable. Here, we report two new molecular phases. The first, $tζ$-N$_2$, is a polytype of monoclinic $C2/c$ $ζ$-N$_2$, characterized by a tripled $c$ axis and 96 atoms per unit cell. The second, $ξ$-N$_2$, is a previously unreported hexagonal phase ($P6cc$) containing 112 atoms per unit cell. Both phases were synthesized in a diamond anvil cell by laser heating $ζ$-N$_2$ to 1800--2500~K at pressures of 78--98~GPa. Their crystal structures were determined using single-crystal X-ray diffraction, corroborated by Raman spectroscopy, and supported by first-principles calculations. The $tζ$-N$_2$ phase likely corresponds to the previously reported $κ$-N$_2$ phase.

cond-mat.mtrl-sci↗

arXiv2026

High-pressure stabilization of Mg2IrH7: Structural proximity to high-Tc superconductivity

Mg$_2$IrH$_6$ is a metastable complex metal hydride with a predicted superconducting transition temperature as high as 170 K at ambient pressure. Following the synthesis of isomorphic, insulating Mg$_2$IrH$_5$ at low pressure, higher-pressure studies were conducted to investigate the phase behavior and compound formation in this system. X-ray diffraction and Raman spectroscopic measurements indicate that cubic Mg$_2$IrH$_7$ is stabilized above ca. 40 GPa and coexists with a related hexagonal hydride with likely composition near Mg$_2$IrH$_5$. Electrical transport measurements show that the cubic Mg$_2$IrH$_7$ is insulating, in agreement with ab initio predictions, and persists during room-temperature decompression until $\sim$20 GPa before reverting back to the cubic Mg$_2$IrH$_5$. The experimental results confirm ground-state structure predictions in the Mg-Ir-H system, and the formation of two nearly identical phases with surrounding compositions opens new opportunities to access superconducting Mg$_2$IrH$_6$ through non-equilibrium processing pathways.

cond-mat.supr-con↗

arXiv2025

Building Wet Planets through High-Pressure Magma-Hydrogen Reactions

Close-in transiting sub-Neptunes are abundant in our galaxy \cite{fulton2017california}. Planetary interior models based on their observed radius-mass relationship suggest that sub-Neptunes contain a discernible amount of either hydrogen (dry planets) or water (wet planets) blanketing a core composed of rocks and metal \cite{bean2021nature}. Water-rich sub-Neptunes have been believed to form farther from the star and then migrate inward to their present orbits \cite{bitsch2021Dry}. Here, we report experimental evidence of reactions between warm dense hydrogen fluid and silicate melt that releases silicon from the magma to form alloys and hydrides at high pressures. We found that oxygen liberated from the silicate melt reacts with hydrogen, producing a significant amount of water up to a few tens of weight percent, which is much greater than previously predicted based on low-pressure ideal gas extrapolation \cite{misener2023Atmospheresa,schlichting2022Chemical}. Consequently, these reactions can generate a spectrum of water contents in hydrogen-rich planets, with the potential to reach water-rich compositions for some sub-Neptunes, implying an evolutionary relationship between hydrogen-rich and water-rich planets. Therefore, detection of a large amount of water in exoplanet atmospheres may not be the optimal evidence for planet migration in the protoplanetary disk, calling into question the assumed link between composition and planet formation location.

astro-ph.EP↗

arXiv2025

X-ray Diffraction and Electrical Transport Imaging of Superconducting Superhydride (La,Y)H10

We report the synthesis and characterization of (La0.9Y0.1)H10 superhydrides exhibiting coexisting cubic Fm-3m and hexagonal P63/mmc clathrate phases observed over the pressure range from 168 GPa down to 136 GPa. Using synchrotron-based X-ray diffraction imaging (XDI) at the upgraded Advanced Photon Source (APS-U), we spatially resolved micron-scale distributions of these phases, revealing structural inhomogeneity across the sample. Four-probe DC resistance measurements confirmed superconductivity, with two distinct transitions: an onset at 244 K associated with the cubic phase and a second near 220 K linked to the hexagonal phase. Notably, resistance profiles collected from different current and voltage permutations showed variations in transition width and onset temperature that correlated with the spatial phase distribution mapped by XDI. These findings demonstrate a direct connection between local structural domains and superconducting behavior. Yttrium substitution is found to influence both the phase behavior and superconducting properties of LaH10-type clathrate hydrides. More broadly, this study highlights the utility of spatially correlating structural and electrical transport measurements in materials exhibiting heterogeneity under pressure, including hydride superconductors.

cond-mat.supr-con↗

arXiv2025

Long-Term Stability of Superconducting Metal Superhydrides

Zhou et al., in their recent publication (Nat. Commun. 16, 1135, 2025), reported the synthesis of lanthanum superhydride, LaHx (x = 10.2-11.1), by laser heating LaH3 with NH3BH3 at a pressure of 170 GPa and investigated the temporal evolution of the NMR spectra of the reaction products. They observed a gradual decrease in the 1H-NMR signal intensity assigned to the synthesized metal hydride, accompanied by an increase in molecular hydrogen within the sample chamber over a period of 50 days. Based on these observations, the authors concluded that LaH10 progressively decomposes into LaH3 and H2 within two months after synthesis at its formation pressure of 170 GPa. Here, we demonstrate that, under their formation conditions, metal superhydrides are thermodynamically more stable than metal trihydrides. Furthermore, we present direct experimental evidence - based on X-ray diffraction and four-probe electrical resistance measurements - confirming the stability of both the crystal lattice and high-temperature superconducting properties of the Fm-3m-LaH10 phase for more than five years. This long-term stability is consistent with predictions from quantum chemistry calculations.

cond-mat.supr-con↗

arXiv2025

Prediction and Synthesis of Mg$_4$Pt$_3$H$_6$: A Metallic Complex Transition Metal Hydride Stabilized at Ambient Pressure

The low-pressure stabilization of superconducting hydrides with high critical temperatures ($T_c$s) remains a significant challenge, and experimentally verified superconducting hydrides are generally constrained to a limited number of structural prototypes. Ternary transition-metal complex hydrides (hydrido complexes)-typically regarded as hydrogen storage materials-exhibit a large range of compounds stabilized at low pressure with recent predictions for high-$T_c$ superconductivity. Motivated by this class of materials, we investigated complex hydride formation in the Mg-Pt-H system, which has no known ternary hydride compounds. Guided by ab initio structural predictions, we successfully synthesized a novel complex transition-metal hydride, Mg$_4$Pt$_3$H$_6$, using laser-heated diamond anvil cells. The compound forms in a body-centered cubic structural prototype at moderate pressures between 8-25 GPa. Unlike the majority of known hydrido complexes, Mg$_4$Pt$_3$H$_6$ is metallic, with formal charge described as 4[Mg]$^{2+}$.3[PtH$_2$]$^{2-}$. X-ray diffraction (XRD) measurements obtained during decompression reveal that Mg$_4$Pt$_3$H$_6$ remains stable upon quenching to ambient conditions. Magnetic-field and temperature-dependent electrical transport measurements indicate ambient-pressure superconductivity with $T_c$ (50%) = 2.9 K, in reasonable agreement with theoretical calculations. These findings clarify the phase behavior in the Mg-Pt-H system and provide valuable insights for transition-metal complex hydrides as a new class of hydrogen-rich superconductors.

cond-mat.supr-con↗

arXiv2025

Hydrogen-rich hydrate at high pressures up to 104 GPa

Gas hydrates are considered fundamental building blocks of giant icy planets like Neptune and similar exoplanets. The existence of these materials in the interiors of giant icy planets, which are subject to high pressures and temperatures, depends on their stability relative to their constituent components. In this study, we reexamine the structural stability and hydrogen content of hydrogen hydrates, (H2O)(H2)n, up to 104 GPa, focusing on hydrogen-rich materials. Using synchrotron single-crystal X-ray diffraction, Raman spectroscopy, and first-principles theoretical calculations, we find that the C2-filled ice phase undergoes a transformation to C3-filled ice phase over a broad pressure range of 47 - 104 GPa at room temperature. The C3 phase contains twice as much molecular H2 as the C2 phase. Heating the C2-filled ice above approximately 1500 K induces the transition to the C3 phase at pressures as low as 47 GPa. Upon decompression, this phase remains metastable down to 40 GPa. These findings establish new stability limits for hydrates, with implications for hydrogen storage and the interiors of planetary bodies.

cond-mat.mtrl-sci↗

arXiv2024

Origin of Pressure-Induced Structural Instability in CsPbX$_3$ Photovoltaic Perovskites

Under external stimuli, lead halide perovskites exhibit large atomic fluctuations, impacting optical and electron transport properties that affect device performance in operational settings. However, a thorough understanding of the atomic basis for the underlying structural instability is still absent. Focusing on the model material CsPbBr$_3$, the inherent lattice softness of halide perovskites is elucidated at the atomic level through in-situ single-crystal X-ray diffraction measurements under pressure complemented by atomic level simulations. We identify and explore the nature of the first-order phase transition to a distorted P21/c phase at 1.3 GPa, induced by the sudden Cs-Br bonds breaking. Unlike classical transition metal oxide perovskites, where the internal energy term dominates, we show explicitly that pressure primarily influences the Gibbs free energy for halide perovskites through the pressure-volume term. As such, strategically mitigating bond strains from volume shrinkage is the key to suppressing the first-order behavior for maintaining the coordinates of PbX$_6$ polyhedral upon external perturbation. Our thermodynamic calculation reveals the demand for high entropy in the -T*del-S term, which can be achieved by exploring a broader spectrum of doped A site and B sites in ABX$_3$ systems, enabling continuous structural changes that facilitate recovery from mechanical damage in practical applications.

cond-mat.mtrl-sci↗

arXiv2024

Phase transition kinetics revealed by in situ X-ray diffraction in laser-heated dynamic diamond anvil cells

We report on a novel approach to dynamic compression of materials that bridges the gap between previous static- and dynamic- compression techniques, allowing to explore a wide range of pathways in the pressure-temperature space. By combining a dynamic-diamond anvil cell setup with double-sided laser-heating and in situ X-ray diffraction, we are able to perform dynamic compression at high temperature and characterize structural transitions with unprecedented time resolution. Using this method, we investigate the $γ-ε$ phase transition of iron under dynamic compression for the first time, reaching compression rates of hundreds of GPa/s and temperatures of 2000 K. Our results demonstrate a distinct response of the $γ-ε$ and $α-ε$ transitions to the high compression rates achieved. These findings open up new avenues to study tailored dynamic compression pathways in the pressure-temperature space and highlight the potential of this platform to capture kinetic effects in a diamond anvil cell.

cond-mat.mtrl-sci↗

arXiv2024

Stability of Hydrides in Sub-Neptune Exoplanets with Thick Hydrogen-Rich Atmospheres

Many sub-Neptune exoplanets have been believed to be composed of a thick hydrogen-dominated atmosphere and a high-temperature heavier-element-dominant core. From an assumption that there is no chemical reaction between hydrogen and silicates/metals at the atmosphere-interior boundary, the cores of sub-Neptunes have been modeled with molten silicates and metals (magma) in previous studies. In large sub-Neptunes, pressure at the atmosphere-magma boundary can reach tens of gigapascals where hydrogen is a dense liquid. A recent experiment showed that hydrogen can induce the reduction of Fe$^{2+}$ in (Mg,Fe)O to Fe$^0$ metal at the pressure-temperature conditions relevant to the atmosphere-interior boundary. However, it is unclear if Mg, one of the abundant heavy elements in the planetary interiors, remains oxidized or can be reduced by H. Our experiments in the laser-heated diamond-anvil cell found that heating of MgO + Fe to 3500-4900 K (close to or above their melting temperatures) in a H medium leads to the formation of Mg$_2$FeH$_6$ and H$_2$O at 8-13 GPa. At 26-29 GPa, the behavior of the system changes, and Mg-H in an H fluid and H$_2$O were detected with separate FeH$_x$. The observations indicate the dissociation of the Mg-O bond by H and subsequent production of hydride and water. Therefore, the atmosphere-magma interaction can lead to a fundamentally different mineralogy for sub-Neptune exoplanets compared with rocky planets. The change in the chemical reaction at the higher pressures can also affect the size demographics (i.e., "radius cliff") and the atmosphere chemistry of sub-Neptune exoplanets.

astro-ph.EP↗

arXiv2023

Efficient Up-Conversion in CsPbBr3 Nanocrystals via Phonon-Driven Exciton-Polaron Formation

Lead halide perovskite nanocrystals demonstrate efficient up-conversion, although the precise mechanism remains a subject of active research. This study utilizes steady-state and time-resolved spectroscopy methods to unravel the mechanism driving the up-conversion process in CsPbBr3 nanocrystals. Employing above- and below-gap photoluminescence measurements, we extract a distinct phonon mode with an energy of ~7 meV and identify the Pb-Br-Pb bending mode as the phonon involved in the up-conversion process. This result was corroborated by Raman spectroscopy. We confirm an up-conversion efficiency reaching up to 75%. Transient absorption measurements under conditions of sub-gap excitation also unexpectedly reveal coherent phonons for the subset of nanocrystals undergoing up-conversion. This coherence implies that the up-conversion and subsequent relaxation is accompanied by a synchronized and phased lattice motion. This study reveals that efficient up-conversion in CsPbBr3 nanocrystals is powered by a unique interplay between the soft lattice structure, phonons, and excited states dynamics.

cond-mat.mtrl-sci↗

arXiv2023

Superconductivity above 180 K in Ca-Mg Ternary Superhydrides at Megabar Pressures

The discovery of high-temperature superconductivity above 240 K in binary La-H and Y-H systems inspired further predictions of even higher transition temperatures in compounds such as YH10 and MgH6, which are likely to be dynamically unstable. Ternary superhydrides provide alternative pathways to stabilize desired near-room temperature superconducting phases. However, the synthesis of new ternary hydrides remains challenging because most of the precursor reactants do not exist in desired stoichiometry at ambient conditions. Here we report that using the existing binary intermetallic CaMg2 and 1:1 Ca-Mg mixture as starting reactants, we have successfully synthesized novel Ca-Mg-based ternary superhydrides at megabar pressures. Electrical resistivity measurements show Tc approaching 168 K at 310 GPa in the CaMg2-based superhydride and 182 K in 1:1 the Ca-Mg superhydride at 324 GPa.

cond-mat.supr-con↗

arXiv2023

Silvanite AuAgTe$_4$: a rare case of gold superconducting material

Gold is one of the most inert metals, forming very few compounds, some with rather interesting properties, and only two of them currently known to be superconducting under certain conditions (AuTe$_2$ and SrAuSi$_3$). Compounds of another noble element, Ag, are also relatively rare, and very few of them are superconducting. Finding new superconducting materials containing gold (and silver) is a challenge - especially having in mind that the best high-$T_c$ superconductors at normal conditions are based upon their rather close ''relative'', Cu. Here we report combined X-ray diffraction, Raman, and resistivity measurements, as well as first-principles calculations, to explore the effect of hydrostatic pressure on the properties of the sylvanite mineral, AuAgTe$_4$. Our experimental results, supported by density functional theory, reveal a structural phase transition at $\sim$5 GPa from a monoclinic $P2/c$ to $P2/m$ phase, resulting in almost identical coordinations of Au and Ag ions, with rather uniform interatomic distances. Further, resistivity measurements show the onset of superconductivity at $\sim$1.5 GPa in the $P2/c$ phase, followed by a linear increase of $T_c$ up to the phase transition, with a maximum in the $P2/m$ phase, and a gradual decrease afterwards. Our calculations indicate phonon-mediated superconductivity, with the electron-phonon coupling coming predominantly from the low-energy phonon modes. Thus, along with the discovery of a new superconducting compound of gold/silver, our results advance understanding of the mechanism of the superconductivity in Au-containing compounds, which may pave the way to the discovery of novel ones.

cond-mat.str-el↗

arXiv2023

Assessing the stability fields of molecular and polymeric CO2

We investigated the stability of polymeric CO2 over a wide range of pressures, temperatures, and chemical environments. We find that the I-42d polymeric structure, consisting of a three-dimensional network of corner sharing CO4 tetrahedra, forms at 40-140 GPa and from a CO-N2 mixture at 39 GPa. An exceptional stability field of 0 to 286 GPa and 100 to 2500 K is documented for this structure, making it a viable candidate for planetary interiors. The stability of the tetrahedral polymeric motif of CO2-V is a consequence of the rigidity of sp3 hybridized orbitals of carbon in a closed-packed oxygen sublattice.

cond-mat.mtrl-sci↗

arXiv2023

Superconductivity above 70 K observed in lutetium polyhydrides

The binary polyhydrides of heavy rare earth lutetium that shares a similar valence electron configuration to lanthanum have been experimentally discovered to be superconductive. The lutetium polyhydrides were successfully synthesized at high pressure and high temperature conditions using a diamond anvil cell in combinations with the in-situ high pressure laser heating technique. The resistance measurements as a function of temperature were performed at the same pressure of synthesis in order to study the transitions of superconductivity (SC). The superconducting transition with a maximum onset temperature (Tc) 71 K was observed at pressure of 218 GPa in the experiments. The Tc decreased to 65 K when pressure was at 181 GPa. From the evolution of SC at applied magnetic fields, the upper critical field at zero temperature μ0Hc2(0) was obtained to be ~36 Tesla. The in-situ high pressure X-ray diffraction experiments imply that the high Tc SC should arise from the Lu4H23 phase with Pm-3n symmetry that forms a new type of hydrogen cage framework different from those reported for previous light rare earth polyhydride superconductors.

cond-mat.supr-con↗

arXiv2023

Observation of Conventional Near Room Temperature Superconductivity in Carbonaceous Sulfur Hydride

The phenomenon of high temperature superconductivity, approaching room temperature, has been realized in a number of hydrogen-dominant alloy systems under high pressure conditions1-12. A significant discovery in reaching room temperature superconductivity is the photo-induced reaction of sulfur, hydrogen, and carbon that initially forms of van der Waals solids at sub-megabar pressures. Carbonaceous sulfur hydride has been demonstrated to be tunable with respect to carbon content, leading to different superconducting final states with different structural symmetries. A modulated AC susceptibility technique adapted for a diamond anvil cell confirms a Tc of 260 kelvin at 133 GPa in carbonaceous sulfur hydride. Furthermore, direct synchrotron infrared reflectivity measurements on the same sample under the same conditions reveal a superconducting gap of ~85 meV at 100 K in close agreement to the expected value from Bardeen-Cooper-Schrieffer (BCS) theory13-18. Additionally, x-ray diffraction in tandem with AC magnetic susceptibility measurements above and below the superconducting transition temperature, and as a function of pressure at 107-133 GPa, reveal the Pnma structure of the material is responsible for the close to room-temperature superconductivity at these pressures.

cond-mat.supr-con↗

arXiv2023

Structural evolution of iodine on approach to the monatomic state

We applied single-crystal X-ray diffraction and Raman spectroscopy in a diamond anvil cell up to 36 GPa and first principles theoretical calculations to study the molecular dissociation of solid iodine at high pressure. Unlike previously reported, we find that the familiar Cmce molecular phase transforms to a Cmc21 molecular structure at 16 GPa, and then to an incommensurate dynamically disordered Fmmm(00γ)s00 structure at 20 GPa, which can be viewed as a stepwise formation of polymeric zigzag chains of three iodine atoms following by the formation of the dynamically dissociated, incommensurately modulated i-Fmmm phase, and the truly monatomic Immm phase at higher pressures.

cond-mat.mtrl-sci↗

arXiv2022

Synthesis of Ultra-Incompressible Carbon Nitrides Featuring Three-Dimensional Frameworks of CN4 Tetrahedra Recoverable at Ambient Conditions

More than thirty years ago, carbon nitrides featuring 3D frameworks of tetrahedral CN4 units were identified as one of the great aspirations of materials science, expected to have a hardness greater than or comparable to diamond. Since then, no unambiguous experimental evidence of their existence has been delivered. Here, we report the high-pressure high-temperature synthesis of the long-sought-after covalent carbon nitrides, tI14-C3N4, hP126-C3N4, and tI24-CN2, in laser-heated diamond anvil cells. Their structures were solved and refined using synchrotron single-crystal X-ray diffraction. In these solids, carbon atoms, all sp3-hybridized, and nitrogen atoms are fully saturated, forming four and three covalent bonds, respectively, leading to three-dimensional arrangements of corner-sharing CN4 tetrahedra. These carbon nitrides are ultra-incompressible, with hP126-C3N4 and tI24-CN2 even rivalling diamond's incompressibility, and superhard. These novel compounds are recoverable to ambient conditions in crystalline form and chemically stable in air. Being wide-band gap semiconductors with intriguing features in their electronic structure, they are expected to exhibit multiple exceptional functionalities besides their mechanical properties, opening new perspectives for materials science.

cond-mat.mtrl-sci↗