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  1. Abstract High pressure is an effective tool to induce exotic quantum phenomena in magnetic topological insulators by controlling the interplay of magnetic order and topological state. This work presents a comprehensive high-pressure study of the crystal structure and magnetic ground state up to 62 GPa in an intrinsic topological magnet EuSn 2 P 2 . With a combination of high resolution X-ray diffraction, 151 Eu synchrotron Mössbauer spectroscopy, X-ray absorption spectroscopy, molecular orbital calculations, and electronic band structure calculations, it has been revealed that pressure drives EuSn 2 P 2 from a rhombohedral crystal to an amorphous phase at 36 GPa accompanied by a fourfold enhancement of magnetic ordering temperature. In the pressure-induced amorphous phase, Eu ions take an intermediate valence state. The drastic enhancement of magnetic ordering temperature from 30 K at ambient pressure to 130 K at 41.2 GPa resulting from Ruderman–Kittel–Kasuya–Yosida (RKKY) interactions likely attributes to the stronger Eu–Sn interaction at high pressure. These rich results demonstrate that EuSn 2 P 2 is an ideal platform to study the correlation of the enhanced RKKY interactions, disordered lattice, intermediate valence, and topological state.
    Free, publicly-accessible full text available December 1, 2023
  2. Formation of vitreous ice during rapid compression of water at room temperature is important for biology and the study of biological systems. Here, we show that Raman spectra of rapidly compressed water at greater than 1 GPa at room temperature exhibits the signature of high-density amorphous ice, whereas the X-ray diffraction (XRD) pattern is dominated by crystalline ice VI. To resolve this apparent contradiction, we used molecular dynamics simulations to calculate full vibrational spectra and diffraction patterns of mixtures of vitreous ice and ice VI, including embedded interfaces between the two phases. We show quantitatively that Raman spectra, which probe the local polarizability with respect to atomic displacements, are dominated by the vitreous phase, whereas a small amount of the crystalline component is readily apparent by XRD. The results of our combined experimental and theoretical studies have implications for detecting vitreous phases of water, survival of biological systems under extreme conditions, and biological imaging. The results provide additional insight into the stable and metastable phases of H 2 O as a function of pressure and temperature, as well as of other materials undergoing pressure-induced amorphization and other metastable transitions.
    Free, publicly-accessible full text available July 5, 2023
  3. Abstract Isotopic fractionation has been linked to the lattice vibrations of materials through their phonon spectra. The Lamb-Mössbauer factor (fLM) has the potential to provide information about the lattice vibrations in materials. We constrain the temperature evolution of the fLM of γ- and ε-Fe at in situ high-P-T conditions between 1650 K and the melting point. We find that the vibrations of γ- and ε-Fe can be described using a quasiharmonic model with a pressure- and temperature-dependent Debye temperature computed from the measured fLM. From the Debye temperature, we derive the equilibrium isotopic fractionation β-factor of iron. Our results show that the quasiharmonic behavior of metallic iron would lower the value of lnβFe57/54 by 0.1‰ at 1600–2800 K and 50 GPa when compared to the extrapolation of room temperature nuclear resonant inelastic X-ray scattering data. Our study suggests that anharmonicity may be more prevalent in Fe metal than in lower mantle minerals at 2800 K and 50 GPa, a relevant condition for the core formation, and the silicate mantle may be isotopically heavy in iron.
    Free, publicly-accessible full text available March 1, 2023
  4. Nanocrystalline olivine-structured Mg2SiO4 and MgCoSiO4, with an average particle size of 27 nm and 31 nm, respectively, were successfully synthesized from oxide precursors via mechanochemical methods. The two nanocrystalline products were obtained after milling for 360 min and displayed high concentrations of Mg2SiO4 (>94%) and MgCoSiO4 (>95%), together with minor amounts of WC (~3%) contaminant originating as debris abraded off milling balls and chambers. The macroscopic temperature monitoring of the grinding jars during milling trials recorded a peak temperature of 75 °C. A combination of analytical techniques that included XRD, TEM, SAED, and EDS were employed for the characterization of the synthesized products.
    Free, publicly-accessible full text available March 1, 2023
  5. Abstract As a major nominally anhydrous mineral (NAM) in the Earth’s upper mantle, orthopyroxene could host up to several hundred parts per million H2O in its crystal structure and transport the H2O to the deep Earth. To study the effect of structural H2O on the elasticity of orthopyroxene, we have measured the single-crystal elasticity of Mg1.991Al0.065Si1.951O6 with 842–900 ppm H2O and 1.64 ± 0.20 wt% Al2O3 at ambient conditions using Brillouin spectroscopy. The best-fit single-crystal elastic moduli (Cijs), bulk (KS0), and shear (G0) modulus of the hydrous Al-bearing orthopyroxene were determined as: C11 = 235(2) GPa, C22 = 173(2) GPa, C33 = 222(2) GPa, C44 = 86(1) GPa, C55 = 82(1) GPa, C66 = 82(1) GPa, C12 = 75(3) GPa, C13 = 67(2) GPa, and C23 = 49(2) GPa, KS0 = 111(2) GPa, and G0 = 78(1) GPa. Systematic analysis based on the results presented in this and previous studies suggests that the incorporation of 842–900 ppm H2O would increase C13 by 12.0(7)% and decrease C23 by 8.6(8)%. The effects on C11, C22, C33, C44, C66, KS0, and VP are subtle if not negligible when considering the uncertainties. The C55, C12, G0, and VS are not affected by the presencemore »of structural H2O. Although laboratory experiments show that Fe,Al-bearing orthopyroxenes can host up to 0.8 wt% H2O in its structure, future high-pressure-temperature elasticity measurements on orthopyroxene with higher H2O content are needed to help better quantify this effect.« less
    Free, publicly-accessible full text available April 1, 2023
  6. Free, publicly-accessible full text available April 1, 2023
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  8. Co 2 SiO 4 is a ceramic pigment and promising battery material of significant technological interest, as well as a model end-member of one of the most important mineral families in the Earth's crust and upper mantle. All previously developed methods for synthesis of Co 2 SiO 4 require high-temperature processing, which promotes grain growth, while the nanocrystalline form is required for some important technological applications. Here, we report a successful method for synthesizing nanocrystalline Co 2 SiO 4 via a simple and inexpensive high-energy ball milling mechanochemical process. Products of the synthesis were characterized by a combination of XRD and TEM, and their crystal structures and elemental compositions are reported.
  9. Abstract

    Earth-abundant antimony trisulfide (Sb2S3), or simply antimonite, is a promising material for capturing natural energies like solar power and heat flux. The layered structure, held up by weak van-der Waals forces, induces anisotropic behaviors in carrier transportation and thermal expansion. Here, we used stress as mechanical stimuli to destabilize the layered structure and observed the structural phase transition to a three-dimensional (3D) structure. We combined in situ x-ray diffraction (XRD), Raman spectroscopy, ultraviolet-visible spectroscopy, and first-principles calculations to study the evolution of structure and bandgap width up to 20.1 GPa. The optical band gap energy of Sb2S3followed a two-step hierarchical sequence at approximately 4 and 11 GPa. We also revealed that the first step of change is mainly caused by the redistribution of band states near the conduction band maximum. The second transition is controlled by an isostructural phase transition, with collapsed layers and the formation of a higher coordinated bulky structure. The band gap reduced from 1.73 eV at ambient to 0.68 eV at 15 GPa, making it a promising thermoelectric material under high pressure.