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  • 1.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Physics.
    Dielectric relaxation of low-density amorphous ice under pressure.2007In: Physical Review Letters, Vol. 98, no 5, p. 057602-Article in journal (Refereed)
  • 2.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Physics.
    Dielectric relaxation of the amorphous ices2008In: J. Phys.: Condens. Matter, Vol. 20Article in journal (Refereed)
    Abstract [en]

    The dielectric properties of the low and high density amorphous ices are discussed in terms of those for supercooled water and crystalline ices, and also used to evaluate the transition

    behaviour upon pressure cycling at 130 K. The dielectric relaxation of the high density amorphous ice is described well by the symmetrical Cole–Cole function with an almost pressure independent relaxation time τ ∼ 2 s at 133 K and a relaxation time distribution factor of 0.7. At the high to low density amorphous ice transition, the dielectric relaxation time increases by about two orders of magnitude despite a ∼30% decrease in density, and τ of the low density amorphous ice is in the range 102–103 s at 130 K. The relaxation time behaviour of

    the high density amorphous ice is similar to that of supercooled liquid water, whereas τ of the low density amorphous ice appears to be prolonged by the ice rules, in correspondence to that

    of the crystalline ices.

  • 3.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Glass-liquid transition of water at high pressure2011In: Proceedings of the National Academy of Sciences of the United States of America, ISSN 0027-8424, E-ISSN 1091-6490, Vol. 108, no 27, p. 11013-11016Article in journal (Refereed)
    Abstract [en]

    The knowledge of the existence of liquid water under extreme conditions and its concomitant properties are important in many fields of science. Glassy water has previously been prepared by hyperquenching micron-sized droplets of liquid water and vapor deposition on a cold substrate (ASW), and its transformation to an ultraviscous liquid form has been reported on heating. A densified amorphous solid form of water, high-density amorphous ice (HDA), has also been made by collapsing the structure of ice at pressures above 1 GPa and temperatures below approximately 140 K, but a corresponding liquid phase has not been detected. Here we report results of heat capacity C(p) and thermal conductivity, in situ, measurements, which are consistent with a reversible transition from annealed HDA to ultraviscous high-density liquid water at 1 GPa and 140 K. On heating of HDA, the Cp increases abruptly by (3.4 ± 0.2) J mol-1 K-1 before crystallization starts at (153 ± 1) K. This is larger than the Cp rise at the glass to liquid transition of annealed ASW at 1 atm, which suggests the existence of liquid water under these extreme conditions.

  • 4.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Physics.
    Relaxation time of water's high-density amorphous ice phase2005In: Physical Review Letters, ISSN 0031-9007, E-ISSN 1079-7114, Physical Review Letters, Vol. 95, no 20, p. 205503-Article in journal (Refereed)
  • 5.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Thermal conductivity of normal and deuterated water, crystalline ice, and amorphous ices2018In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 149, no 12, article id 124506Article in journal (Refereed)
    Abstract [en]

    The effect of deuteration on the thermal conductivity kappa of water, crystalline ice, and amorphous ices was studied using the pressure induced amorphization of hexagonal ice, ice Ih, to obtain the deuterated, D2O, forms of low-density amorphous (LDA), high-density amorphous (HDA), and very-high density amorphous (VHDA) ices. Upon deuteration, kappa of ice Ih decreases between 3% and 4% in the 100-270 K range at ambient pressure, but the effect diminishes on densification at 130 K and vanishes just prior to amorphization near 0.8 GPa. The unusual negative value of the isothermal density rho dependence of kappa for ice Ih, g = (d ln kappa/d ln rho)(T) = -4.4, is less so for deuterated ice: g = -3.8. In the case of the amorphous ices and liquid water, kappa of water decreases by 3.5% upon deuteration at ambient conditions, whereas K of HDA and VHDA ices instead increases by up to 5% for pressures up to 1.2 GPa at 130 K, despite HDA's and VHDA's structural similarities with water. The results are consistent with significant heat transport by librational modes in amorphous ices as well as water, and that deuteration increases phonon-phonon scattering in crystalline ice. Heat transport by librational modes is more pronounced in D2O than in H2O at low temperatures due to a deuteration-induced red-shift of librational mode frequencies. Moreover, the results show that kappa of deuterated LDA ice is 4% larger than that of normal LDA at 130 K, and both forms display an unusual temperature dependence of kappa, which is reminiscent of that for crystals (kappa similar to T (-1)), and a unique negative pressure dependence of kappa, which likely is linked to local-order structural similarities to ice Ih. 

  • 6.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Carvalho, Paulo H. B. Brant
    Hsu, Ying-Jui
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Haussermann, Ulrich
    Transitions in pressure-amorphized clathrate hydrates akin to those of amorphous ices2019In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 151, no 1, article id 014502Article in journal (Refereed)
    Abstract [en]

    Type II clathrate hydrates (CHs) were studied by thermal and dielectric measurements. All CHs amorphize, or collapse, on pressurization to 1.3 GPa below 135 K. After heating to 160 K at 1 GPa, the stability of the amorphous states increases in a process similar to the gradual high density to very high density amorphous ice (HDA to VHDA) transition. On a subsequent pressure decrease, the amorphized CHs expand partly irreversibly similar to the gradual VHDA to expanded HDA ice transformation. After further heating at 1 GPa, weak transition features appear near the HDA to low density amorphous ice transition. The results suggest that CH nucleation sites vanish on heating to 160 K at 1 GPa and that a sluggish partial phase-separation process commences on further heating. The collapsed CHs show two glass transitions (GTs), GT1 and GT2. GT1 is weakly pressure-dependent, 12 K GPa(-1), with a relaxation time of 0.3 s at 140 K and 1 GPa; it is associated with a weak heat capacity increase of 3.7 J H2O-mol(-1) K-1 in a 18 K range and an activation energy of only 38 kJ mol(-1) at 1 GPa. The corresponding temperature of GT2 is 159 K at 0.4 GPa with a pressure dependence of 36 K GPa(-1); it shows 5.5 times larger heat capacity increase and 4 times higher activation energy than GT1. GT1 is observed also in HDA and VHDA, whereas GT2 occurs just above the crystallization temperature of expanded HDA and only within its similar to 0.2-0.7 GPa stable pressure range.

  • 7.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Chobal, O.
    Rizak, I.
    Rizak, V.
    Sabadosh, V.
    Effects of pressure and temperature on the thermal conductivity of Sn2P2S62011In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 83, no 13, article id 134121Article in journal (Refereed)
    Abstract [en]

    The thermal conductivity kappa of the ferroelectric, paraelectric, and incommensurate phases of polycrystalline Sn2P2S6 has been measured in the 0.1-0.7 GPa range. The thermal conductivity kappa of the ferroelectric phase decreases with increasing pressure p. This unusual behavior, which is found in only a few other phases, is attributed to a negative Gruneisen parameter. The temperature T dependence of kappa for the ferroelectric phase (kappa similar to T-1) is well described by the Debye model for kappa, with three-phonon Umklapp scattering serving as the dominant scattering mechanism near and above the Debye temperature (similar to 100 K) up to a few tenths of degrees below the ferro- to paraelectric phase transition, where kappa(T) gradually changes and becomes temperature independent upon further heating. The thermal conductivity of the paraelectric and incommensurate phases was temperature independent and indistinguishable. Possible causes for the unusually weak T dependence at high temperatures and implications of the p dependence of kappa are discussed.

  • 8.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Chobal, Oleksandr
    Department of Solid State Electronics, Uzhhorod National University, Ukraine.
    Rizak, I
    Department of Integrated Technologies of Aviation Manufacture, National Aerospace University of “KhAI", Kharkov, Ukraine.
    Rizak, V
    Department of Solid State Electronics, Uzhhorod National University, Ukraine.
    Tricritical Lifshitz point in the temperature-pressure-composition diagram for (PbySn1-y)2 P2(SexS1-x)6 ferroelectrics2009In: Physical Review B Condensed Matter, ISSN 0163-1829, E-ISSN 1095-3795, Vol. 80, p. 174107-Article in journal (Refereed)
    Abstract [en]

    The heat capacity of Sn2P2S6 ferroelectric crystals has been measured under quasihydrostatic pressures up to 0.7 GPa. The analysis of the heat-capacity and literature data for the birefringence shows that the tricritical point of Sn2P2S6 is in the 0.20–0.25 GPa range. Moreover, in the approximation of a linear change in the free-energy expansion coefficients, with respect to concentration and pressure, thermodynamic trajectories have been constructed for (PbySn1−y)2 P2(SexS1−x)6 solid solutions. We have thereby identified the region of the T-p-y-x diagram for (PbySn1−y)2 P2(SexS1−x)6 showing the tricritical Lifshitz point.

  • 9.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Filinchuk, Yaroslav
    Dmitriev, Vladimir
    Quwar, Issam
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Talyzin, Alexandr
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sundqvist, Bertil
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Phase coexistence and hysteresis effects in the pressure-temperature phase diagram of NH3BH32011In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 84, no 2, p. 024115-Article in journal (Refereed)
    Abstract [en]

    The potential hydrogen storage compound NH3BH3 has three known structural phases in the temperature and pressure ranges 110–300 K and 0–1.5 GPa, respectively. We report here the boundaries between, and the ranges of stability of, these phases. The phase boundaries were located by in situ measurements of the thermal conductivity, while the actual structures in selected areas were identified by in situ Raman spectroscopy and x-ray diffraction. Below 0.6 GPa, reversible transitions involving only small hysteresis effects occur between the room-temperature tetragonal plastic crystal I4mm phase and the low-temperature orthorhombic Pmn21 phase. Transformations of the I4mm phase into the high-pressure orthorhombic Cmc21 phase, occurring above 0.8 GPa, are associated with very large hysteresis effects, such that the reverse transition may occur at up to 0.5 GPa lower pressures. Below 230 K, a fraction of the Cmc21 phase is metastable to atmospheric pressure, suggesting the possibility that dense structural phases of NH3BH3, stable at room temperature, could possibly be created and stabilized by alloying or by other methods. Mixed orthorhombic Pmn21/Cmc21 phases were observed in an intermediate pressure-temperature range, but a fourth structural phase predicted by Filinchuk et al. [ Phys. Rev. B 79 214111 (2009)] was not observed in the pressure-temperature ranges of this experiment. The thermal conductivity of the plastic crystal I4mm phase is about 0.6 W m−1 K−1 and only weakly dependent on temperature, while the ordered orthorhombic phases have higher thermal conductivities limited by phonon-phonon scattering.

  • 10.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Häussermann, Ulrich
    A Second Glass Transition in Pressure Collapsed Type II Clathrate Hydrates2018In: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 122, no 15, p. 4376-4384Article in journal (Refereed)
    Abstract [en]

    Type II clathrate hydrates (CHs) M·17 H2O, with M = tetrahydrofuran (THF) or 1,3-dioxolane, are known to collapse, or amorphize, on pressurization to ∼1.3 GPa in the temperature range 77–140 K. On heating at 1 GPa, these pressure-amorphized CH states show a weak, stretched sigmoid-shaped, heat-capacity increase because of a glass transition. Here we use thermal conductivity and heat capacity measurements to show that also type II CH with M = cyclobutanone (CB) collapses on isothermal pressurization and undergoes a similar, weak, glass transition upon heating at 1 GPa. Furthermore, we reveal for both THF CH and CB CH a second, much more pronounced, glass transition at temperatures above the thermally weak glass transition on heating in the 0.2–0.7 GPa range. This result suggests the general occurrence of two glass transitions in water-rich (94 mol %) pressure-collapsed CHs. Because of a large increase in dielectric permittivity concurrently as the weak heat capacity increase, the first glass transition must be due to kinetic unfreezing of water molecules. The thermal features of the second glass transition, measured on isobaric temperature cycling, are typical of a glass–liquid–glass transition, which suggests that pressure-amorphized CHs transform reversibly to liquids.

  • 11.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Physics.
    Inaba, Akira
    Dielectric properties of the high-density amorphous ice under pressure2006In: Physical Review B, Vol. 74, no 18, p. 184201-Article in journal (Refereed)
  • 12.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Inaba, Akira
    Research Center for Structural Thermodynamics, Graduate School of Science, Osaka University, Japan.
    Glass Transitions in Pressure-Collapsed Ice Clathrates and Implications for Cold Water2012In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 3, no 15, p. 1951-1955Article in journal (Refereed)
    Abstract [en]

    Ice is known to collapse to amorphous ice upon pressurization at low temperatures and shows the unusual feature of multiple distinct solid amorphous water states, which have inspired models of liquid water’s structure and unusual properties.Here, we use heat capacity Cp measurements to show that similarly collapsed ice clathrates display identical glass behavior as amorphous ice but that crystallization above the glass transition temperature Tg of ∼140 K at 1 GPa is inhibited. This effect of the homogeneously distributed “guest molecules” in water reveals a relatively strong reversible Cp increase above Tg but no further transition before crystallization at ∼190 K.This is consistent with a glass−liquid transition of water at Tg, which suggests a new path to study an ultraviscous liquid water network and evaluate water models

  • 13.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Physics.
    Inaba, Akira
    Thermal conductivity of crystalline and amorphous ices and its implications on amorphization and glassy water2005In: Physical Chemistry Chemical Physics, Vol. 7, p. 1441-Article in journal (Refereed)
  • 14.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Inaba, Akira
    Unusual Grüneisen and Bridgman parameters of low-density amorphous ice and their implications on pressure induced amorphization2005In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 122, no 12, p. 124710-Article in journal (Refereed)
    Abstract [en]

    The low-temperature limiting value of the Grüneisen parameter for low-frequency phonons and the density dependence of the thermal conductivity (Bridgman parameter) of low-density amorphous (LDA) ice, high-density amorphous (HDA) ice, hexagonal ice Ih, and cubic ice Ic were calculated from high-pressure sound velocity and thermal conductivity measurements, yielding negative values for all states except HDA ice. LDA ice is the first amorphous state to exhibit a negative Bridgman parameter, and negative Grüneisen parameters are relatively unusual. Since Ih, Ic, and LDA ice all transform to HDA upon pressurization at low temperatures and share the unusual feature of negative Grüneisen parameters, this seems to be a prerequisite for pressure induced amorphization. We estimate that the Grüneisen parameter increases at the ice Ih to XI transition, and may become positive in ice XI, which indicates that proton-ordered ice XI does not amorphize like ice Ih on pressurization.

  • 15.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Johari, G P
    Sub-Tg features of glasses formed by cooling glycerol under pressure – Additional incompatibility of vibrational with configurational states in the depressurized, high density glass2016In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 145, article id 204506Article in journal (Refereed)
    Abstract [en]

    The vibrational state of a glass is naturally incompatible with its configurational state, which makes the glass structurally unstable. When a glass is kept at constant temperature, both the vibrational and configurational states of a glass change with time until it becomes metastable (equilibrium) liquid and the two states become compatible. The process, known as structural relaxation, occurs at a progressively higher rate during heating, and the properties of a glass change accordingly. We add to this incompatibility by depressurizing a glass that had been formed by cooling a liquid under a high pressure, p, and then investigate the effects of the added incompatibility by studying thermal conductivity, κ, and the heat capacity per unit volume ρCp of the depressurized glass.We use glycerol for the purpose and study first the changes in the features of κ and of ρCp during glass formation oncooling under a set of different p. We then partially depressurize the glass and study the effect of the p-induced instability on the features of and Cp as the glass is isobarically heated to the liquid state.At a given low p, the glass configuration that was formed by cooling at high-p had a higher κ than the glass configuration that was formed by cooling at a low p. The difference is more when the glass is formed at a higher p and/or is depressurized to a lower p. On heating at a low p, its κ decreases before its glass-liquid transition range is reached. The effect is the opposite of the increase in observed on heating a glass at the same p under which it was formed. It is caused by thermally assisted loss of the added incompatibility of configurational and vibrational states of a high-p formed glass kept at low p. If a glass formed under a low-p is pressurized and then heated under high p, it would show the opposite effect, i.e., its κ would first increase to its high p value before its glass-to-liquid transition range.

  • 16.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Physics.
    Johari, G.P
    Shanker, R.M.
    Effect of pressure on molecular and ionic motions in ultraviscous acetaminophen-aspirin mixture2006In: Journal of Pharmaceutical Sciences, Vol. 95, p. 2406-Article in journal (Refereed)
  • 17.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Physics.
    Johari, Gyan P.
    Collapse of an ice clathrate under pressure observed via thermal conductivity measurements2008In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 78, p. 174201-Article in journal (Refereed)
    Abstract [en]

    Irreversible transformation of the tetrahydrofuran ice clathrate at 130 K was studied by measuring thermal conductivity k with increase in pressure p. Initially, k increases slowly with p up to 0.75 GPa where it levels off, is roughly constant up to 0.95 GPa, then decreases up to 1.05 GPa. Pressure collapses the clathrate structure, plausibly beginning with lattice distortion, and k increases at 1.05 GPa in a sharp sigmoid-shape manner due to large densification until the transformation is complete at 1.25 GPa. This is the opposite of that found for ice whose k decreases first slowly with increase in p and then rapidly in an inverted sigmoidshape manner [O. Andersson and H. Suga, Phys. Rev. B 65, 140201 (2002)]. At 1.08 GPa and 131 K, k increases with time t (s) according to exp(t /2945), which is also the opposite of the collapse of ice [G. P. Johari and O. Andersson, Phys. Rev. B 70, 184108 (2004)]. The difference in its behavior is attributed to strong phonon scattering from the tetrahydrofuran guest molecules. k of the collapsed clathrate is 30% less than that for the collapsed ice, which is comparable with the 25% lesser k of the tetrahydrofuran-water solution from k of water at ambient pressure. On depressurizing at 130 K, k decreases progressively more rapidly and k of the collapsed state at 0.3 GPa is slightly lower than that of the as-made clathrate, showing that its original structure is not recovered.

  • 18.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Johari, Gyan P
    Effect of pressure on thermal conductivity and pressure collapse of ice in a polymer-hydrogel and kinetic unfreezing at 1 GPa2011In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 134, no 12, p. 124903-Article in journal (Refereed)
    Abstract [en]

    We report a study of aqueous solutions of poly(vinylalcohol) and its hydrogel by thermal conductivity,κ, and specific heat measurements. In particular, we investigate (i) the changes in the solution and the hydrogel at 0.1 MPa observed in the 350-90 K range and of the frozen hydrogel at 130 K observed in the range from 0.1 MPa to 1.3 GPa, and (ii) the nature of the pressure collapse of ice in the frozen hydrogel and kinetic unfreezing on heating of its high density water at 1 GPa. The water component of the polymer solution on cooling either first phase separates and then freezes to hexagonal ice or freezes without phase separation and the dispersed polymer chains freeze-concentrate in nanoscopic and microscopic regions of the grain boundaries and grain junctions of the ice crystals in the frozen state of water in the hydrogel. The change in κ with temperature at 1 bar is reversible with some hysteresis, but not reversible with pressure after compression to 0.8 GPa at 130 K. At high pressures the crystallized state collapses showing features of. and specific heat characteristic of formation of high density amorphous solid water. The pressure of structural collapse is 0.08 GPa higher than that of ice at 130 K. The slowly formed collapsed state shows kinetic unfreezing or glass-liquid transition temperature at 140 K for a time scale of 1 s. Comparison with the change in the properties observed for ice shows that κ decreases when the polymer is added. 

  • 19.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Physics. Umeå University, Faculty of Science and Technology, Physics.
    Johari, Gyan P.
    Nature of the pressure-induced collapse of an ice clathrate by dielectric spectroscopy2008In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 129, p. 234505-Article in journal (Refereed)
    Abstract [en]

    Collapse of an ice clathrate of type II structure containing tetrahydrofuran as guest molecules has been studied at different pressures by dielectric spectroscopy. The sample was pressurized to 1.3 GPa at 130 K and the resulting collapsed state was pressure cycled. The dielectric relaxation time increases at a progressively rapid rate during pressurizing and then decreases slowly on depressurizing, but the dielectric relaxation time does not reach the value of the original state. With increase in pressure, the limiting high frequency permittivity due to orientation of H2O molecules first increases by about 5% until 0.75 GPa and then decreases slightly until 1 GPa, and finally it increases until ~1.2 GPa. The decrease is attributed to the loss of contribution from the reorientational motion of tetrahydrofuran molecules and the increase to densification as the structure mechanically collapses completely in the 1–1.25 GPa range. The relaxation time of the collapsed state is comparable with that of the high-density amorph formed on pressure collapse of ice.

  • 20.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Johari, Gyan P
    Department of Materials Science and Engineering, McMaster University, Hamilton, Canada.
    Pressure-induced collapse of ice clathrate and hexagonal ice mixtures formed by freezing2009In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 131, p. 114503-114513Article in journal (Refereed)
    Abstract [en]

    We report thermal conductivity κ measurements of the pressure-induced collapse of two mixtures of ice and tetrahydrofuran (THF) clathrate hydrate formed by freezing aqueous solutions, THF·23 H2O and THF·20 H2O, one containing twice as much excess water than the other. On pressurizing, κ of the solid mixture first decreases at the onset pressure of 0.8 GPa, as occurs for collapse of pure ice, reaches a local minimum at a pressure of 1.0 GPa, and then increases as occurs for the collapse of the pure clathrate THF·17 H2O. This shows that in the apparently homogeneous mixture, the ice and the clathrate collapse as if the two were in a mechanically mixed state. The manner in which the clathrate aggregate can arrange in the solid indicates that ice occupies the interstitial space in the tightly packed aggregates and H2O molecules belonging to the lattice of one form hydrogen bond with that of the other, a feature that is preserved in their collapsed states. On decompression, the original clathrate is partially recovered in the THF·20 H2O mixture, but the collapsed ice does not transform to the low density amorph. We surmise that on irreversible transformation to the original clathrate, the aggregates expand. Any pressure thus exerted on the small domains of the collapsed ice with a hydrogen bonded interface with the clathrate aggregates could prevent it from transforming to the low density amorph. Measurements of κ are useful in investigating structural collapse of crystals when dilatometry is unable to do so, as κ seems to be more sensitive to pressure-induced changes than the volume.

  • 21.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Johari, Gyan P
    Spontaneous transformation of water's high-density amorph and a two-stage crystallization to ice VI at 1 GPa: a dielectric study2004In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 120, no 24, p. 11662-11671Article in journal (Refereed)
    Abstract [en]

    Dielectric relaxation spectra of a metastable crystal phase formed on implosive and exothermic transformation of pressure-amorphized hexagonal ice have been measured in situ at 0.97 GPa pressure over a range of temperature. The metastable phase showed no relaxation peak at 130 K and 0.97 GPa. When heated at a fixed pressure of 0.97 GPa, it began to transform at ∼ 145 K exothermally to a phase whose relaxation rate and equilibrium dielectric permittivity increased. A second, but slower exothermic transformation also occurred at ∼ 175 K. After keeping at 213 K, the relaxation rate and equilibrium permittivity reached the known values of these two quantities for ice VI. Thus the metastable phase transformed to ice VI in two stages. It is conjectured that the intermediate phase in this transformation could be ice XII. The rate of transformation is not determined by the reorientational relaxation rate of water molecules in the ices

  • 22.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Johari, Gyan P.
    Department of Materials Science and Engineering, McMaster University, Hamilton, Ontario, Canada.
    Thermal conductivity of Glycerol’s liquid, glass, and crystal states, glass-liquid-glass transition, and crystallization at high pressures2016In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 144, article id 064504Article in journal (Refereed)
  • 23.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Johari, Gyan P
    Time-dependent amorphization of ice at 0.8-0.9 GPa2004In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 121, no 8, p. 3936-3938Article in journal (Refereed)
    Abstract [en]

    Thermal conductivity measurements show that ice continues to amorphize for several days when kept at a fixed pressure p in the 0.79–0.88 GPa range, and fixed temperature T in the 127–130 K range. Thermal conductivity k decreases according to a stretched exponential in time, and its limiting long time value k() varies with p and T. At 0.8 GPa and 128 K, k() remains 2.5 times the value observed for high-density amorph. Consequences of these findings for our understanding of amorphization are discussed.

  • 24.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Johari, Gyan P
    Suga, H.
    An ice phase of lowest thermal conductivity2004In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 120, no 20, p. 9612-9617Article in journal (Refereed)
    Abstract [en]

    On pressurizing at temperatures near 130 K, hexagonal and cubic ices transform implosively at 0.8–1 GPa. The phase produced on transformation has the lowest thermal conductivity among the known crystalline ices and its value decreases on increase in temperature. An ice phase of similar thermal conductivity is produced also when high-density amorphous ice kept at 1 GPa transforms on slow heating when the temperature reaches ∼155 K. These unusual formation conditions, the density and its distinguished thermal conductivity, all indicate that a distinct crystal phase of ice has been produced.

  • 25.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Nakazawa, Yasuhiro
    Transitions in pressure collapsed clathrate hydrates2015In: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 119, no 9, p. 3846-3853Article in journal (Refereed)
    Abstract [en]

    Type II clathrate hydrates (CHs), or ice clathrates, are inclusion compounds in which a hydrogen-bonded cage-like structure of H2O accommodates molecules of suitable size, known as guest molecules. CHs have similar local geometrical arrangements of the hydrogen-bonded water network as ice and both are known to collapse to amorphous states on isothermal pressurization at temperatures below about 140 K. Moreover, the collapsed CH states undergo a glass, or glass-like, transition at 140 K on heating at 1 GPa, which is identical to that of collapsed ice, or high density amorphous ice. Here we use thermal conductivity and dielectric measurements to study the transition behavior of two type II CHs with tetrahydrofuran and 1,3 dioxolane, respectively, as guest molecules. After their collapsed states have been heated to well above the glass transition at 1 GPa, we find transitions corresponding to the high to low density amorphous ice transition of ice with only slightly shifted temperature-pressure (T-p) coordinates compared to those of pure water. Thus, collapsed CHs show the same transition behaviors as cold water, which provide the basis for the model that explains the unusual temperature and pressure behaviors of waters properties in terms of two distinct types of liquid water. Collapsed CHs are, however, more stable than collapsed ice and can therefore be studied in a wider T-p interval. The results suggest sluggish homogenizing and phase separation processes, which affect the transition behaviors of collapsed CHs.

  • 26.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Physics.
    Ostrovskii, D.
    Jacobsson, Per
    A high pressure study of PMMA-based gels with and without TiO2 nano-particle filler: A filler induced change in the activation volume2005In: Electrochimica Acta, Vol. 50, p. 3217-Article in journal (Refereed)
  • 27.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Physics.
    Soldatov, Alexander
    Umeå University, Faculty of Science and Technology, Physics.
    Sundqvist, Bertil
    Umeå University, Faculty of Science and Technology, Physics.
    Reorientational relaxation in C60 following a pressure induced change in the pentagon/hexagon equilibrium ratio1995In: Physics Letters A, ISSN 0375-9601, E-ISSN 1873-2429, Vol. 206, no 3-4, p. 260-264Article in journal (Refereed)
    Abstract [en]

    The orientational structure of C60 depends on pressure and temperature. Pressurization below the glass transition temperature Tg can freeze in non-equilibrium orientational structures. The relaxation of such structures on heating through Tg has been studied through thermal conductivity measurements and the effects observed are explained in a simple model.

  • 28.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Physics.
    Soldatov, Alexander
    Umeå University, Faculty of Science and Technology, Physics.
    Sundqvist, Bertil
    Umeå University, Faculty of Science and Technology, Physics.
    Thermal conductivity of C60 at pressures up to 1 GPa and temperatures in the range 50-300 K1996In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 54, no 5, p. 3093-3100Article in journal (Refereed)
    Abstract [en]

    The thermal conductivity λ of C60 shows anomalies near 260 K and 90 K which are associated with the well-established phase transition and glass transition, respectively. Both transition temperatures increase with pressure, at the rates 120 K GPa-1 and 62 K GPa-1, respectively. With increasing temperature, λ of the simple cubic (sc) phase increased below 170 K (glasslike behavior) but decreased above. The glasslike behavior of λ is probably due to a substantial amount of lattice defects. Possible reasons for the change of sign of dλ/dT near 170 K are discussed. In the face centered cubic (fcc) phase (T≳260 K at atmospheric pressure) λ was almost independent of temperature, a behavior which is far from that of an ordered crystal (λ∝T-1 for T≳Debye temperature). This result can be attributed to the molecular orientational disorder of the fcc phase. The relaxation behavior associated with the glassy state and its unusually strong dependence on thermal history are discussed briefly, and data which support a previously reported relaxation model are presented. At room temperature, the density dependencies of λ, (∂ lnλ/∂ lnρ)T, were 5.5 and 9.5 for the fcc and sc phases, which are values typical for an orientationally disordered phase and a normal crystal phase, respectively.

  • 29.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Physics.
    Soldatov, Alexander
    Umeå University, Faculty of Science and Technology, Physics.
    Sundqvist, Bertil
    Umeå University, Faculty of Science and Technology, Physics.
    Thermal conductivity of C60 under high pressure1995In: Science and Technology of Fullerene Materials: Materials Research Society Symposium Proceedings vol. 359, Pittsburgh, PA: Materials Research Society , 1995, p. 549-554Conference paper (Refereed)
    Abstract [en]

    We have measured the thermal conductivity lambda of highly pure polycrystalline C60 in the range 50 to 300 K under pressures up to 1 GPa. The results are discussed in terms of the lattice structure and dynamics. In particular, we discuss the phase diagram as delineated by anomalies observed in lambda and cp at the f.c.c.-to-s.c. transition at 260 K and the glass transition at Tg = 90 K, and also the effect on lambda of the orientational motion in the s.c. phase. The results are found to be compatible with a p/T phase diagram recently suggested by us.

  • 30.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Physics.
    Suga, H.
    On the unusual thermal conductivity of ices at elevated pressures2005In: Netsu Sokutei (Japan), Vol. 32, no 5, p. 232-Article, review/survey (Other (popular science, discussion, etc.))
  • 31.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Physics.
    Sundqvist, Bertil
    Umeå University, Faculty of Science and Technology, Physics.
    Bäckström, Gunnar
    Umeå University, Faculty of Science and Technology, Physics.
    A low-temperature high-pressure apparatus with a temperature control system1992In: High Pressure Research, ISSN 0895-7959, E-ISSN 1477-2299, Vol. 10, no 4, p. 599-606Article in journal (Refereed)
    Abstract [en]

    A low-temperature high-pressure apparatus was designed using commercial cryogenic equipment. Pressures up to 1 GPa and temperatures down to 40 K can be obtained in a volume of up to 30 cm3. The apparatus is of the piston-cylinder type with a piston diameter of 45 mm, and the pressure can be varied at all temperatures, An adaptive temperature control system keeps the temperature inside the pressure cylinder constant to within ±0.1 K.

  • 32.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Physics.
    Wågberg, Thomas
    Umeå University, Faculty of Science and Technology, Physics.
    In situ, high pressure differential thermal analysis and ionic conductance of PMMA-based gels with and without TiO2 nano-particle filler2006In: Electrochimica Acta, Vol. 51, p. 4537-Article in journal (Refereed)
  • 33.
    Andersson, Ove
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Yasuhiro, Nakazawa
    Research Center for Structural Thermodynamics, Graduate School of Science, Osaka University, Toyonaka, Osaka 560-0043, Japan.
    Thermal Properties and Transition Behavior of Host –Guest Compounds under High Pressure2014In: Current inorganic chemistry, ISSN 1877-9441, Vol. 4, no 1, p. 2-18Article in journal (Other academic)
    Abstract [en]

    The thermal properties and transition behavior of the host-guest inclusion compounds: urea, thiourea, Dianin’s compound, clathrate hydrates and hydroquinone have been reviewed. In particular, we summarize their thermal conductivities, heat capacities and transitions at high pressures. Two of the systems: urea inclusion compounds and clathrate hydrates, show unusual glass-like thermal conductivity k, i.e. their k is low and only weakly dependent on temperature  despite their crystalline structure. Moreover, results for k of Dianin’s compound with guests such as ethanol and CCl4 indicate a change from glass-like k  at atmospheric pressure to crystalline-like k at elevated pressure, whereas k of hydroquinone and thiourea inclusion compounds appears not to have been studied. Despite the technological and fundamental importance of the unusual glass-like k, e.g. the use of inclusion compounds as structural model systems for finding improved thermoelectrical materials, the origin of the glass-like k is not established. More specifically, the commonly employed rattling model, in which rattling guest motions cause resonance scattering of the acoustic host phonons, has recently been challenged, and we discuss alternative models. Heat capacity studies of these compounds reveal numerous transitions, which are associated with guest and host disorder-order transitions upon cooling and pressurization. A transition in hydroquinone may be of second order, or have only a small first-order component, which can explain discrepancies in the observed transition behavior. On pressurization at low temperatures, clathrate hydrates collapse to an amorphous state, which appears to be a glassy state of a water solution with perfectly spaced solute molecules.

  • 34. Bair, Scott S.
    et al.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Qureshi, Farrukh S.
    Schirru, Michele M.
    New EHL Modeling Data for the Reference Liquids Squalane and Squalane Plus Polyisoprene2018In: Tribology Transactions, ISSN 1040-2004, E-ISSN 1547-397X, Vol. 61, no 2, p. 247-255Article in journal (Refereed)
    Abstract [en]

    An important part of the new quantitative approach to elastohydrodynamic lubrication (EHL) is the use of reference liquids with well-characterized thermophysical properties. New measurements are reported for the thermal and rheological properties of squalane to high pressure and of high shear rate and high-frequency viscosity of squalane thickened with polyisoprene (SQL + PIP) at ambient pressure. The glass transition viscosity of squalane at ambient pressure was found from published viscosity measurements and new glass transition measurements by transient hot wire. The glass transition viscosity so determined was incorporated into the improved Yasutomi model and the calculated glass transition temperatures as a function of pressure are comparable to those directly measured, although the hybrid model yields better agreement. The glass transition viscosity of squalane by any definition must be substantially lower than the “universal value” of 1012 Pa·s. The second Newtonian inflection cannot be characterized in steady shear at ambient pressure for SQL + PIP due to cavitation; however, acoustic viscometry with matching layer does characterize the second Newtonian inflection. To form the analogy between steady and oscillatory shear requires that the steady shear rate be compared with the ordinary frequency rather than the angular frequency for SQL + PIP.

  • 35. Carvalho, Paulo H. B. Brant
    et al.
    Mace, Amber
    Bull, Craig L.
    Funnell, Nicholas P.
    Tulk, Chris A.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Häussermann, Ulrich
    Elucidation of the pressure induced amorphization of tetrahydrofuran clathrate hydrate2019In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 150, no 20, article id 204506Article in journal (Refereed)
    Abstract [en]

    The type II clathrate hydrate (CH) THF·17 H2O (THF = tetrahydrofuran) is known to amorphize on pressurization to ∼1.3 GPa in the temperature range 77–140 K. This seems to be related to the pressure induced amorphization (PIA) of hexagonal ice to high density amorphous (HDA) ice. Here, we probe the PIA of THF-d8 · 17 D2O (TDF-CD) at 130 K by in situthermal conductivity and neutron diffraction experiments. Both methods reveal amorphization of TDF-CD between 1.1 and 1.2 GPa and densification of the amorphous state on subsequent heating from 130 to 170 K. The densification is similar to the transition of HDA to very-high-density-amorphous ice. The first diffraction peak (FDP) of the neutron structure factor function, S(Q), of amorphous TDF-CD at 130 K appeared split. This feature is considered a general phenomenon of the crystalline to amorphous transition of CHs and reflects different length scales for D-D and D-O correlations in the water network and the cavity structure around the guest. The maximum corresponding to water-water correlations relates to the position of the FDP of HDA ice at ∼1 GPa. Upon annealing, the different length scales for water-water and water-guest correlations equalize and the FDP in the S(Q) of the annealed amorph represents a single peak. The similarity of local water structures in amorphous CHs and amorphous ices at in situ conditions is confirmed from molecular dynamics simulations. In addition, these simulations show that THF guest molecules are immobilized and retain long-range correlations as in the crystal.

  • 36. Dmitriev, Vladimir
    et al.
    Filinchuk, Yaroslav
    Chernyshov, Dmitry
    Talyzin, Alexandr
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Dzwilewski, Andrzej
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sundqvist, Bertil
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Kurnosov, Alexander
    Pressure-temperature phase diagram of LiBH4: Synchrotron x-ray diffraction experiments and theoretical analysis2008In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 77, no 17, article id 174112Article in journal (Refereed)
    Abstract [en]

    An in situ combined high-temperature high-pressure synchrotron radiation diffraction study has been carried out on LiBH4. The phase diagram of LiBH4 is mapped to 10 GPa and 500 K, and four phases are identified. The corresponding structural distortions are analyzed in terms of symmetry-breaking atomic position shifts and anion ordering. Group-theoretical and crystal-chemical considerations reveal a nontrivial layered structure of LiBH4. The layers and their deformations define the structural stability of the observed phases.

  • 37.
    Habchi, W
    et al.
    Department of Industrial and Mechanical Engineering, Lebanese American University (LAU), Byblos, Lebanon.
    Vergne, P
    Université de Lyon, CNRS, INSA-Lyon, LaMCoS UMR5259, Villeurbanne, France.
    Bair, Scott
    G.W. Woodruff School of Mechanical Engineering, Centre for High-Pressure Rheology, Georgia Institute of Technology, Atlanta, GA.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Eyheramendy, D
    Department of Industrial and Mechanical Engineering, Lebanese American University (LAU), Byblos, Lebanon.
    Morales-Espejel, G.E.
    SKF Engineering and Research Center, Nieuwegein, The Netherlands.
    Influence of pressure and temperature dependence of thermal properties of a lubricant on the behaviour of circular TEHD contacts2010In: Tribology International, ISSN 0301-679X, E-ISSN 1879-2464, Vol. 43, no 10, p. 1842-1850Article in journal (Refereed)
    Abstract [en]

    The aim of this paper is to study the effects of pressure and temperature dependence of a conventional lubricant's thermal properties on the behaviour of heavily loaded thermal elastohydrodynamic lubrication (TEHL) contacts. For this purpose, a typical mineral oil (Shell T9) is selected and the dependence of its transport properties on pressure and temperature is investigated. Appropriate models are then developed for these dependencies. The latter are included in a TEHL solver in order to investigate their effect on the behaviour of circular EHD contacts. The results reveal the necessity of a thermal analysis including the pressure and temperature dependence of thermal properties for a good estimation of film thicknesses and mostly traction coefficients in circular EHD contacts operating under severe conditions. Numerical results are compared with experiments, showing a very good agreement over the considered ranges. This thorough validation of a thermal EHL framework for the calculation of film thickness and friction offers a previously unavailable opportunity to investigate the effects of variations in material properties.

  • 38. Inaba, Akira
    et al.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Physics.
    Multiple glass transitions and two step crystallization for the binary system of water and glycerol2007In: Thermochimica Acta 461, issue 1-2, 2007, p. 44-49Conference paper (Refereed)
    Abstract [en]

    Glass formation/crystallization phenomena were studied in water and glycerol mixtures using adiabatic calorimetry. The sample was cooled rapidly from room temperature and its thermal response was followed on heating from 80 to 300 K. The binary mixtures with the glycerol contents more than 55% (w/w) (19 mol%) yielded the homogeneous glassy states, consisting of randomly mixed water and glycerol molecules. Their glass transition temperatures showed the composition dependence of the Gordon-Taylor equation, and extrapolated exactly to that of pure water (135 K). The mixtures in the 0-55% (w/w) glycerol range crystallized partly on cooling and exhibited three anomalies in the temperature drift rate on heating. The first of these three is associated with the onset of reorientational motions of water molecules in the hexagonal ice which increases from 107 to 120 K on increasing the glycerol composition. The second is the composition independent temperature of 164 K that corresponds to the mixture with 76% (w/w) glycerol (38 mol%, known as the maximally freeze-concentrated solution), which is the mixture with the maximum composition of water that can be cooled without crystallization. The third is associated with the ice crystallization followed by ice dissolution in the range 185-202 K. In addition, the sample with 60% (w/w) glycerol composition (23 mol%) exhibited two distinguishable exothermic peaks on heating. The initial one is large and is attributed to crystallization into a novel two-dimensionally ordered structure of ice, and the second is due to the transformation of the layered structures into the hexagonal ice.

  • 39. Johari, G. P.
    et al.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Effects of stacking disorder on thermal conductivity of cubic ice2015In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 143, no 5, article id 054505Article in journal (Refereed)
    Abstract [en]

    Cubic ice is said to have stacking disorder when the H2O sequences in its structure (space group Fd (3) over barm) are interlaced with hexagonal ice (space group P6(3)/mmc) sequences, known as stacking faults. Diffraction methods have shown that the extent of this disorder varies in samples made by different methods, thermal history, and the temperature T, but other physical properties of cubic and hexagonal ices barely differ. We had found that at 160 K, the thermal conductivity, kappa, of cubic ice is similar to 20% less than that of hexagonal ice, and this difference varies for cubic ice samples prepared by different methods and/or subjected to different thermal history. After reviewing the methods of forming cubic ice, we report an investigation of the effects of stacking disorder and other features by using new data, and by analyzing our previous data on the dependence of kappa on T and on the pressure. We conclude that the lower kappa of cubic ice and its weaker T-dependence is due mainly to stacking disorder and small crystal sizes. On in situ heating at 20-50 MPa pressure, kappa increases and cubic ice irreversibly transforms more sharply to ice Ih, and at a higher T of similar to 220 K, than it does in ex situ studies. Cooling and heating between 115 and 130 K at 0.1 K min(-1) rate yield the same kappa value, indicating that the state of cubic ice in these conditions does not change with time and T. The increase in kappa of cubic ice observed on heat-annealing before its conversion to hexagonal ice is attributed to the loss of stacking faults and other types of disorders, and to grain growth. After discussing the consequences of our findings on other properties, we suggest that detailed studies of variation of a given property of cubic ice with the fraction of stacking faults in its structure may reveal more about the effect of this disorder. A similar disorder may occur in the mono-layers of H2O adsorbed on a substrate, in bulk materials comprised of two dimensional layers, in diamond and in Zirconium and in numerous other crystals.

  • 40. Johari, G P
    et al.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Physics. Umeå University, Faculty of Science and Technology, Physics.
    In situ transformation of amorphous ices at high pressures2007In: Physical Review B, Vol. 76, p. 134103-1Article in journal (Refereed)
    Abstract [en]

    By using thermal conductivity and its change with temperature and pressure as a criteria for in situ structural transformation of the crystalline and amorphous solid forms of water, we report two findings: (i) transformation of high-density amorph (HDA) directly to cubic ice on slow depressurization and (ii) slow transformation or dilation of metastable HDA at 130 K to a low-density amorph (LDA) even when the pressure was increased from 0.2 to 0.3 GPa, and then gradual reversion by collapse of the LDA to HDA on further pressurization to 0.5 GPa. We also discuss implications of these findings for the current understanding of the transformations of metastable ices under pressure, particularly of those studied in situ.

  • 41. Johari, G. P.
    et al.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Structural relaxation and thermal conductivity of high-pressure formed, high-density di-n-butyl phthalate glass and pressure induced departures from equilibrium state2017In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 146, no 23, article id 234505Article in journal (Refereed)
    Abstract [en]

    We report a study of structural relaxation of high-density glasses of di-n-butyl phthalate (DBP) by measuring thermal conductivity, κ, under conditions of pressure and temperature (p,T) designed to modify both the vibrational and configurational states of a glass. Various high-density glassy states of DBP were formed by (i) cooling the liquid under a fixed high p and partially depressurizing the glass, (ii) isothermal annealing of the depressurized glass, and (iii) pressurizing the glass formed by cooling the liquid under low p. At a given low p, κ of the glass formed by cooling under high p is higher than that of the glass formed by cooling under low p, and the difference increases as glass formation p is increased. κ of the glass formed under 1 GPa is ∼20% higher at ambient p than κ of the glass formed at ambient p. On heating at low p, κ decreases until the glass to liquid transition range is reached. This is the opposite of the increase in κ observed when a glass formed under a certain p is heated under the same p. At a given high p, κ of the low-density glass formed by cooling at low p is lower than that of the high-density glass formed by cooling at that high p. On heating at high p, κ increases until the glass to liquid transition range is reached. The effects observed are due to a thermally assisted approach toward equilibrium at p different from the glass formation p. In all cases, the density, enthalpy, and entropy would change until the glasses become metastable liquids at a fixed p, thus qualitatively relating κ to variation in these properties.

  • 42. Johari, G. P.
    et al.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Sundqvist, Bertil
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Instability and thermal conductivity of pressure-densified and elastically altered orientational glass of Buckminsterfullerene2018In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 148, no 14, article id 144502Article in journal (Refereed)
    Abstract [en]

    We report on the temperature, pressure and time (T, p and t)- dependent features of thermal conductivity, k, of partially ordered, non-equilibrium state of C60-OG, the orientational glass of Buckminsterfullerene (at T below the orientational freezing temperature Tog) made more unstable (i) by partially depressurizing its high-p formed state to elastically expand it, and (ii) by further pressurizing that state to elastically contract it. The sub-Tog effects observed on heating of C60-OG differ from those of glasses, because phonon propagation depends on the ratio of two well-defined orientational states of C60 molecules and the density of the solid. A broad peak-like feature appears at T near Tog in the k-T plots of C60-OG formed at 0.7 and heated at 0.2 GPa, which we attribute to partial overlap of the sub-Tog and Tog features. A sub-Tog local minimum appears in the k -T plots at T well below Tog  of C60-OG formed at 0.1 GPa and heated at 0.5 GPa, and corresponds to the state of maximum disorder. Although Buckminsterfullerene is regarded as an orientationally-disordered crystal, variation of its properties with T and p is qualitatively different from other such crystals. We discuss the findings in terms of the nature of its disorder, sensitivity of its rotational dynamics to temperature and the absence of the Johari-Goldstein relaxation. All seem to affect the phenomenology of its glass-like transition.

  • 43. Johari, G.P.
    et al.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Physics.
    Mechanisms for pressure- and time-dependent amorphization of ice under pressure2004In: Physical Review B, Vol. 70, no 18, p. 184108-Article in journal (Refereed)
  • 44. Johari, G.P.
    et al.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Physics.
    On the nonlinear variation of dc conductivity with dielectric relaxation time2006In: Journal of Chemical Physics, Vol. 125, no 12, p. 124501-Article in journal (Refereed)
  • 45. Johari, G.P.
    et al.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Physics.
    Vibrational and relaxational properties of crystalline and amorphous ices2007In: Thermochimica Acta 461, issue 1-2, 2007, p. 14-43Conference paper (Refereed)
    Abstract [en]

    Pure water forms 15 crystalline ices at different temperatures and pressures, and its solutions containing small molecules form three crystallographically distinct clathrates. Its vapours deposited on a substrate at T< 100K produce a porous amorphous solid and pure water vitrifies (T-g = 136 K) when hyperquenched in micron-size droplets. At a temperature below 140 K, hexagonal and cubic ice collapse when pressure exceeds similar to 1 GPa to a similar to 30% denser amorphous solid, which on heating at ambient pressure transforms to an amorphous solid with density similar to that of hexagonal ice. In this essay, we describe (i) the thermal conductivity of the ices and clathrates and the thermal conductivity and heat capacity of water's amorphous solids, their thermodynamic paths and their transformations, and (ii) the dielectric relaxation time of ultraviscous water formed on heating the amorphous solids. We also describe the characteristics of pressure collapse and subsequent amorphization of hexagonal and cubic ices that occurs over a period of several days according to a stretched exponential kinetics and a pressure-, and temperature-dependent rate constant. This process is attributed to the production of lattice faults during deformation of the ice and the consequent distribution of the Born instability pressures. This ultimately produces a kinetically unstable high-energy amorphs in the same manner as random deformation of crystals produces kinetically unstable high-energy amorphs, with density and properties depending upon their temperature-pressure-time history. On heating at 1 GPa pressure, the pressure-amorphized solid relaxes to a lower energy state, becoming ultraviscous water at 140 K. But on heating at ambient pressure, it irreversibly transforms slowly to a low-density amorph that differs from glassy water and vapour-deposited amorphous solid.

  • 46. Johari, G.P.
    et al.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Physics.
    Vibrational features of water’s amorph at high pressures2006In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 73, no 9, p. 094202-Article in journal (Refereed)
  • 47. Johari, Gyan P
    et al.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Water's polyamorphic transitions and amorphization of ice under pressure2004In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 120, no 13, p. 6207-6213Article in journal (Refereed)
    Abstract [en]

    Transformations of water’s high density amorph (HDA) to low density amorph (LDA) and of LDA’s to cubic ice (Ic) have been studied by in situ thermal conductivity κ measurements at high pressures. The HDA to LDA transformation is unobservable at p of 0.07 GPa, indicating that, for a fixed heating rate, an increase in pressure increases the temperature of HDA to LDA transformation and decreases that of LDA to ice Ic, causing thereby the two transformations to merge, and HDA appears to convert directly to ice Ic. Thus either LDA forms but converts extremely rapidly to ice Ic, or LDA does not form. At a fixed p and T, in the range of pressure amorphization of hexagonal ice, κ continues to decrease with time. Therefore, the amorphization of ice Ih is kinetically controlled. When HDA at 1 GPa was heated from 130 to 157 K and densified to very HDA, its κ increased by 3%. Our findings and a scrutiny of earlier reports show that a reversible transition between HDA and LDA does not occur at ∼135 K and ∼0.2 GPa. Since there is no unique HDA, it is difficult to justify the conjecture for a second critical point for water.

  • 48. Krivchikov, Alexander I.
    et al.
    Andersson, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Thermal Conductivity of Triphenyl Phosphite's Liquid, Glassy, and Glacial States2016In: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 120, no 10, p. 2845-2853Article in journal (Refereed)
    Abstract [en]

    The thermal conductivity kappa and heat capacity per unit volume rho C-p of triphenyl phosphite (TPP) were measured under different pressure and temperature conditions, and with time during the sluggish liquid to glacial state transformation at temperatures about 15 K above the glass transition temperature. As the transformation slowly proceeds during several hours, rho C-p decreases monotonically from that of the liquid state to a value close to that of the vitrified state. Concurrently, kappa increases nonmonotonically with an intermediate local maximum followed by a minimum, before the final rise to a higher kappa. The properties of the ultimately formed glacial state depend on the thermal history, which implies that the state formed under these conditions is a heterogeneous mixture of nanocrystals and mainly amorphous-like solid, and that the relative amount and microstructure depend on the conditions of the transformation. The nonmonotonic changes in phonon propagation during the liquid to glacial transformation suggest microstructural changes which are consistent with a liquid-liquid transformation and sluggish growth of nanocrystals within amorphous-like solid domains. The isobaric thermal conductivity of the as-formed glacial state shows a reversible step increase, just prior to crystallization on heating, which deviates from the typical behavior of glasses, liquids, and crystals. An increase in pressure shifts the step to higher temperatures and suppresses crystallization, which reveals another reversible rise in kappa and C-p. These results show that increased molecular mobility in the glacial state increases and suggest reduced thermal resistance at boundaries or that the motions carry heat.