All Publications

  • The high-pressure lithium-palladium and lithium-palladium-hydrogen systems. Scientific reports Frost, M., McBride, E. E., Smith, J. S., Glenzer, S. H. 2022; 12 (1): 12341


    The lithium-palladium and lithium-palladium-hydrogen systems are investigated at high pressures at and above room temperature. Two novel lithium-palladium compounds are found below [Formula: see text]. An ambient temperature phase is tentatively assigned as [Formula: see text], with [Formula: see text] Aat 8.64 GPa, isostructural with [Formula: see text]. The other phase occurs at high-temperature and is [Formula: see text], [Formula: see text] Aat 3.88 GPa and 200 [Formula: see text], similar to [Formula: see text], which is also known at high pressure. The presence of hydrogen in the system results in an [Formula: see text] structure with [Formula: see text] Aat 9.74 GPa. This persists up to [Formula: see text], the highest pressure studied. Below [Formula: see text] an fcc phase with a large unit cell, [Formula: see text] Aat 0.39 GPa, is also observed in the presence of hydrogen. On heating the hydrogen containing system at 4 GPa the [Formula: see text] phases persists to the melting point of lithium. In both systems melting the lithium results in the loss of crystalline diffraction from palladium containing phases. This is attributed to dissolution of the palladium in the molten lithium, and on cooling the palladium remains dispersed.

    View details for DOI 10.1038/s41598-022-16694-2

    View details for PubMedID 35853930

  • Ultrafast visualization of incipient plasticity in dynamically compressed matter. Nature communications Mo, M., Tang, M., Chen, Z., Peterson, J. R., Shen, X., Baldwin, J. K., Frost, M., Kozina, M., Reid, A., Wang, Y., E, J., Descamps, A., Ofori-Okai, B. K., Li, R., Luo, S., Wang, X., Glenzer, S. 2022; 13 (1): 1055


    Plasticity is ubiquitous and plays a critical role in material deformation and damage; it inherently involves the atomistic length scale and picosecond time scale. A fundamental understanding of the elastic-plastic deformation transition, in particular, incipient plasticity, has been a grand challenge in high-pressure and high-strain-rate environments, impeded largely by experimental limitations on spatial and temporal resolution. Here, we report femtosecond MeV electron diffraction measurements visualizing the three-dimensional (3D) response of single-crystal aluminum to the ultrafast laser-induced compression. We capture lattice transitioning from a purely elastic to a plastically relaxed state within 5 ps, after reaching an elastic limit of~25 GPa. Our results allow the direct determination of dislocation nucleation and transport that constitute the underlying defect kinetics of incipient plasticity. Large-scale molecular dynamics simulations show good agreement with the experiment and provide an atomic-level description of the dislocation-mediated plasticity.

    View details for DOI 10.1038/s41467-022-28684-z

    View details for PubMedID 35217665

  • High Pressure Brillouin Spectroscopy and X-ray Diffraction of Cerium Dioxide MATERIALS Frost, M., Lazarz, J. D., Levitan, A. L., Prakapenka, V. B., Sun, P., Tkachev, S. N., Yang, H., Glenzer, S. H., Gleason, A. E. 2021; 14 (13)


    Simultaneous high-pressure Brillouin spectroscopy and powder X-ray diffraction of cerium dioxide powders are presented at room temperature to a pressure of 45 GPa. Micro- and nanocrystalline powders are studied and the density, acoustic velocities and elastic moduli determined. In contrast to recent reports of anomalous compressibility and strength in nanocrystalline cerium dioxide, the acoustic velocities are found to be insensitive to grain size and enhanced strength is not observed in nanocrystalline CeO2. Discrepancies in the bulk moduli derived from Brillouin and powder X-ray diffraction studies suggest that the properties of CeO2 are sensitive to the hydrostaticity of its environment. Our Brillouin data give the shear modulus, G0 = 63 (3) GPa, and adiabatic bulk modulus, KS0 = 142 (9) GPa, which is considerably lower than the isothermal bulk modulus, KT0∼ 230 GPa, determined by high-pressure X-ray diffraction experiments.

    View details for DOI 10.3390/ma14133683

    View details for Web of Science ID 000670971500001

    View details for PubMedID 34279253

  • High-Pressure Melt Curve and Phase Diagram of Lithium. Physical review letters Frost, M., Kim, J. B., McBride, E. E., Peterson, J. R., Smith, J. S., Sun, P., Glenzer, S. H. 2019; 123 (6): 065701


    We investigate the phase diagram of lithium at temperatures of 200 to 400 K, to pressures over 100 GPa using x-ray diffraction in diamond anvil cells, covering the region in which the melting curve is disputed. To overcome degradation of the diamond anvils by dense lithium we utilize a rapid compression scheme taking advantage of the high flux available at modern synchrotrons. Our results show the hR1 and cI16 phases to be stable to higher temperature than previously reported. The melting minima of lithium is found to be close to room temperature between 40 and 60 GPa, below which the solid is crystalline. Analysis of the stability fields of the cI16 and oC88 phases suggest the existence of a triple point between these and an undetermined solid phase at 60 GPa between 220 and 255 K.

    View details for DOI 10.1103/PhysRevLett.123.065701

    View details for PubMedID 31491150

  • High-Pressure Melt Curve and Phase Diagram of Lithium PHYSICAL REVIEW LETTERS Frost, M., Kim, J. B., McBride, E. E., Peterson, J., Smith, J. S., Sun, P., Glenzer, S. H. 2019; 123 (6)
  • Reactivity of lithium and platinum at elevated densities PHYSICAL REVIEW B Binns, J., Marques, M., Dalladay-Simpson, P., Turnbull, R., Frost, M., Gregoryanz, E., Howie, R. T. 2019; 99 (22)
  • Unusually complex phase of dense nitrogen at extreme conditions NATURE COMMUNICATIONS Turnbull, R., Hanfland, M., Binns, J., Martinez-Canales, M., Frost, M., Marques, M., Howie, R. T., Gregoryanz, E. 2018; 9: 4717


    Nitrogen exhibits an exceptional polymorphism under extreme conditions, making it unique amongst the elemental diatomics and a valuable testing system for experiment-theory comparison. Despite attracting considerable attention, the structures of many high-pressure nitrogen phases still require unambiguous determination. Here, we report the structure of the elusive high-pressure high-temperature polymorph ι-N2 at 56 GPa and ambient temperature, determined by single crystal X-ray diffraction, and investigate its properties using ab initio simulations. We find that ι-N2 is characterised by an extraordinarily large unit cell containing 48 N2 molecules. Geometry optimisation favours the experimentally determined structure and density functional theory calculations find ι-N2 to have the lowest enthalpy of the molecular nitrogen polymorphs that exist between 30 and 60 GPa. The results demonstrate that very complex structures, similar to those previously only observed in metallic elements, can become energetically favourable in molecular systems at extreme pressures and temperatures.

    View details for DOI 10.1038/s41467-018-07074-4

    View details for Web of Science ID 000449627800012

    View details for PubMedID 30413685

    View details for PubMedCentralID PMC6226474

  • Characterization of defect clusters in ion-irradiated tungsten by X-Ray diffuse scattering JOURNAL OF NUCLEAR MATERIALS Sun, P., Wang, Y., Frost, M., Schoenwaelder, C., Levitan, A. L., Mo, M., Chen, Z., Hastings, J. B., Tynan, G. R., Glenzer, S. H., Heimann, P. 2018; 510: 322–30
  • Simultaneous 8.2 keV phase-contrast imaging and 24.6 keV X-ray diffraction from shock-compressed matter at the LCLS APPLIED PHYSICS LETTERS Seiboth, F., Fletcher, L. B., McGonegle, D., Anzellini, S., Dresselhaus-Cooper, L. E., Frost, M., Galtier, E., Goede, S., Harmand, M., Lee, H. J., Levitan, A. L., Miyanishi, K., Nagler, B., Nam, I., Ozaki, N., Roedel, M., Schropp, A., Spindloe, C., Sun, P., Wark, J. S., Hastings, J., Glenzer, S. H., McBride, E. E. 2018; 112 (22)

    View details for DOI 10.1063/1.5031907

    View details for Web of Science ID 000433963500013

  • Understanding the adsorption process in ZIF-8 using high pressure crystallography and computational modelling NATURE COMMUNICATIONS Hobday, C. L., Woodall, C. H., Lennox, M. J., Frost, M., Kamenev, K., Duren, T., Morrison, C. A., Moggach, S. A. 2018; 9: 1429


    Some porous crystalline solids change their structure upon guest inclusion. Unlocking the potential of these solids for a wide variety of applications requires full characterisation of the response to adsorption and the underlying framework-guest interactions. Here, we introduce an approach to understanding gas uptake in porous metal-organic frameworks (MOFs) by loading liquefied gases at GPa pressures inside the Zn-based framework ZIF-8. An integrated experimental and computational study using high-pressure crystallography, grand canonical Monte Carlo (GCMC) and periodic DFT simulations has revealed six symmetry-independent adsorption sites within the framework and a transition to a high-pressure phase. The cryogenic high-pressure loading method offers a different approach to obtaining atomistic detail on guest molecules. The GCMC simulations provide information on interaction energies of the adsorption sites allowing to classify the sites by energy. DFT calculations reveal the energy barrier of the transition to the high-pressure phase. This combination of techniques provides a holistic approach to understanding both structural and energetic changes upon adsorption in MOFs.

    View details for DOI 10.1038/s41467-018-03878-6

    View details for Web of Science ID 000429794300022

    View details for PubMedID 29650966

    View details for PubMedCentralID PMC5897325

  • Equation of state and electron localisation in fcc lithium JOURNAL OF APPLIED PHYSICS Frost, M., Levitan, A. L., Sun, P., Glenzer, S. 2018; 123 (6)

    View details for DOI 10.1063/1.5020296

    View details for Web of Science ID 000425192500031

  • Deformation-aided segregation of Fe -S liquid from olivine under deep Earth conditions: Implications for core formation in the early solar system PHYSICS OF THE EARTH AND PLANETARY INTERIORS Berg, M. L., Bromiley, G. D., Butler, I. B., Frost, M., Bradley, R., Carr, J., Le Godec, Y., Montesi, L. J., Zhu, W., Miller, K., Perrillat, J., Mariani, E., Tatham, D., Redfern, S. T. 2017; 263: 38–54
  • Formation of xenon-nitrogen compounds at high pressure SCIENTIFIC REPORTS Howie, R. T., Turnbull, R., Binns, J., Frost, M., Dalladay-Simpson, P., Gregoryanz, E. 2016; 6: 34896


    Molecular nitrogen exhibits one of the strongest known interatomic bonds, while xenon possesses a closed-shell electronic structure: a direct consequence of which renders both chemically unreactive. Through a series of optical spectroscopy and x-ray diffraction experiments, we demonstrate the formation of a novel van der Waals compound formed from binary Xe-N2 mixtures at pressures as low as 5 GPa. At 300 K and 5 GPa Xe(N2)2-I is synthesised, and if further compressed, undergoes a transition to a tetragonal Xe(N2)2-II phase at 14 GPa; this phase appears to be unexpectedly stable at least up to 180 GPa even after heating to above 2000 K. Raman spectroscopy measurements indicate a distinct weakening of the intramolecular bond of the nitrogen molecule above 60 GPa, while transmission measurements in the visible and mid-infrared regime suggest the metallisation of the compound at ~100 GPa.

    View details for DOI 10.1038/srep34896

    View details for Web of Science ID 000385351500001

    View details for PubMedID 27748357

    View details for PubMedCentralID PMC5066244

  • Novel high-pressure nitrogen phase formed by compression at low temperature PHYSICAL REVIEW B Frost, M., Howie, R. T., Dalladay-Simpson, P., Goncharov, A. F., Gregoryanz, E. 2016; 93 (2)