Ice XI

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Crystal structure of Ice XI viewed along the c-axis Ice XI View along c axis.png
Crystal structure of Ice XI viewed along the c-axis

Ice XI is the hydrogen-ordered form of Ih, the ordinary form of ice. Different phases of ice, from ice II to ice XIX, have been created in the laboratory at different temperatures and pressures. The total internal energy of ice XI is about one sixth lower than ice Ih, so in principle it should naturally form when ice Ih is cooled to below 72  K. The low temperature required to achieve this transition is correlated with the relatively low energy difference between the two structures. [1] Water molecules in ice Ih are surrounded by four semi-randomly directed hydrogen bonds. Such arrangements should change to the more ordered arrangement of hydrogen bonds found in ice XI at low temperatures, so long as localized proton hopping is sufficiently enabled; a process that becomes easier with increasing pressure. [2] Correspondingly, ice XI is believed to have a triple point with hexagonal ice and gaseous water at (~72 K, ~0 Pa).

Contents

Properties

Crystal structure of ice XI (c-axis in the vertical direction) Ice XI side view.png
Crystal structure of ice XI (c-axis in the vertical direction)

Ice XI has an orthorhombic structure with space group Cmc21 containing eight molecules per unit cell. Its lattice parameters are a=4.465(3) Å, b=7.859(4) Å, and c=7.292(2) Å at 5 K. [3] [4] There are actually 16 crystallographically inequivalent hydrogen-ordered configurations of ice with an orthorhombic structure of eight atoms per unit cell, but electronic structure calculations show Cmc21 to be the most stable. [5] [6] Another possible configuration, with space group Pna21 is also of interest, as it is an antiferroelectric crystal, which Davidson and Morokuma incorrectly suggested as the most stable structure in 1984. [7]

In practice, ice XI is most easily prepared from a dilute (10 mM) KOH solution kept just below 72 K for about a week (for D2O a temperature just below 76 K will suffice). [8] [9] The hydroxide ions create defects in the hexagonal ice, allowing protons to jump more freely between the oxygen atoms (and so this structure of ice XI breaks the 'ice rules'). More specifically, each hydroxide ion creates a Bjerrum L defect and an ionized vertex. Both the defect and the ion can move throughout the lattice and 'assist' with proton reordering. The positive K+ ion may also play a role because it is found that KOH works better than other alkali hydroxides. [10] The exact details of these ordering mechanisms are still poorly understood and under question because experimentally the mobility of the hydroxide and K+ ions appear to be very low around 72 K. [11] [12] The current belief is that KOH acts only to assist with the hydrogen reordering and is not required for the lower-energy stability of ice XI. However, calculations by Toshiaki Iitaka in 2010 call this into question. [13] Iitaka argues that the KOH ions compensate for the large net electric dipole moment of the crystal lattice along the c-axis. The aforementioned electronic structure calculations are done assuming an infinite lattice and ignore the effects of macroscopic electric fields created by surface charges. Because such fields are present in any finite size crystal, in non-doped ice XI, domains of alternating dipole moment should form as in conventional ferroelectrics. [13] It has also been suggested that the ice Ih => ice XI transition is enabled by the tunneling of protons. [14]

Although ice XI is thought to be a more stable conformation than ice Ih, the transformation is very slow. According to one report, in Antarctic conditions it is estimated to take at least 100,000 years to form without the assistance of catalysts.[ citation needed ] Ice XI was sought and found in Antarctic ice that was about 100 years old in 1998. [15] A further study in 2004 was not able to reproduce this finding, however, after studying Antarctic ice which was around 3000 years old. [16] The 1998 Antarctic study also claimed that the transformation temperature (ice XI => ice Ih) is −36 °C (237 K), which is far higher than the temperature of the expected triple point mentioned above (72 K, ~0 Pa). Ice XI was also found in experiments using pure water at very low temperature (~10 K) and low pressure – conditions thought to be present in the upper atmosphere. [17] Recently, small domains of ice XI were found to form in pure water; its phase transition back to ice Ih occurred at 72 K while under hydrostatic pressure conditions of up to 70 MPa. [18]

Ice Ih that has been transformed to ice XI and then back to ice Ih, on raising the temperature, retains some hydrogen-ordered domains and more easily transforms back to ice XI again. [19] A neutron powder diffraction study found that small hydrogen-ordered domains can exist up to 111 K. [20]

There are distinct differences in the Raman spectra between ices Ih and XI, with ice XI showing much stronger peaks in the translational (~230 cm−1), librational (~630 cm−1) and in-phase asymmetric stretch (~3200 cm−1) regions. [21] [22]

Ice Ic also has a proton-ordered form. The total internal energy of ice XIc was predicted as similar as ice XIh [23]

History

Hints of hydrogen-ordering in ice had been observed as early as 1964, when Dengel et al. attributed a peak in thermo-stimulated depolarization (TSD) current to the existence of a proton-ordered ferroelectric phase. [24] However, they could not conclusively prove that a phase transition had taken place, and Onsager pointed out that the peak could also arise from the movement of defects and lattice imperfections. Onsager suggested that experimentalists look for a dramatic change in heat capacity by performing a careful calorimetric experiment. A phase transition to ice XI was first identified experimentally in 1972 by Shuji Kawada and others. [25] [26] [27]

Ferroelectric properties

Ice XI is ferroelectric, meaning that it has an intrinsic polarization. To qualify as a ferroelectric it must also exhibit polarization switching under an electric field, which has not been conclusively demonstrated but which is implicitly assumed to be possible. Cubic ice also has a ferrolectric phase and in this case the ferroelectric properties of the ice have been experimentally demonstrated on monolayer thin films. [28] In a similar experiment, ferroelectric layers of hexagonal ice were grown on a platinum (111) surface. The material had a polarization that had a decay length of 30 monolayers suggesting that thin layers of ice XI can be grown on substrates at low temperature without the use of dopants. [29] One-dimensional nano-confined ferroelectric ice XI was created in 2010. [30]

Astrophysical implications

As was mentioned, ice XI can theoretically form at low pressures at temperatures between 50–70 K – temperatures present in astrophysical environments of the outer solar system and within permanently shaded polar craters on the Moon and Mercury. Ice XI forms most easily around 70 K – paradoxically, it takes longer to form at lower temperatures. Extrapolating from experimental measurements, it is estimated to take ~50 years to form at 70 K and ~300 million years at 50 K. [31] It is theorized to be present in places like the upper atmospheres of Uranus and Neptune [20] and on Pluto and Charon. [31]

Small domains of ice XI could exist in the atmospheres of Jupiter and Saturn as well. [20] The fact that small domains of ice XI can exist at temperatures up to 111 K has some scientists speculating that it may be fairly common in interstellar space, with small 'nucleation seeds' spreading through space and converting regular ice, much like the fabled ice-nine mentioned in Vonnegut's Cat's Cradle . [20] [32] The possible roles of ice XI in interstellar space [31] [33] and planet formation [34] have been the subject of several research papers. Until observational confirmation of ice XI in outer space is made, the presence of ice XI in space remains controversial owing to the aforementioned criticism raised by Iitaka. [13] The infrared absorption spectra of ice XI was studied in 2009 in preparation for searches for ice XI in space. [35]

Related Research Articles

<span class="mw-page-title-main">Hydrogen bond</span> Intermolecular attraction between a hydrogen-donor pair and an acceptor

In chemistry, a hydrogen bond is primarily an electrostatic force of attraction between a hydrogen (H) atom which is covalently bonded to a more electronegative "donor" atom or group (Dn), and another electronegative atom bearing a lone pair of electrons—the hydrogen bond acceptor (Ac). Such an interacting system is generally denoted Dn−H···Ac, where the solid line denotes a polar covalent bond, and the dotted or dashed line indicates the hydrogen bond. The most frequent donor and acceptor atoms are the period 2 elements nitrogen (N), oxygen (O), and fluorine (F).

<span class="mw-page-title-main">Ice</span> Frozen water: the solid state of water

Ice is water that is frozen into a solid state, typically forming at or below temperatures of 0 °C, 32 °F, or 273.15 K. As a naturally occurring crystalline inorganic solid with an ordered structure, ice is considered to be a mineral. Depending on the presence of impurities such as particles of soil or bubbles of air, it can appear transparent or a more or less opaque bluish-white color.

In chemistry, hydronium (hydroxonium in traditional British English) is the common name for the cation [H3O]+, also written as H3O+, the type of oxonium ion produced by protonation of water. It is often viewed as the positive ion present when an Arrhenius acid is dissolved in water, as Arrhenius acid molecules in solution give up a proton (a positive hydrogen ion, H+) to the surrounding water molecules (H2O). In fact, acids must be surrounded by more than a single water molecule in order to ionize, yielding aqueous H+ and conjugate base. Three main structures for the aqueous proton have garnered experimental support: the Eigen cation, which is a tetrahydrate, H3O+(H2O)3, the Zundel cation, which is a symmetric dihydrate, H+(H2O)2, and the Stoyanov cation, an expanded Zundel cation, which is a hexahydrate: H+(H2O)2(H2O)4. Spectroscopic evidence from well-defined IR spectra overwhelmingly supports the Stoyanov cation as the predominant form. For this reason, it has been suggested that wherever possible, the symbol H+(aq) should be used instead of the hydronium ion.

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Potassium hydroxide is an inorganic compound with the formula KOH, and is commonly called caustic potash.

The self-ionization of water (also autoionization of water, and autodissociation of water, or simply dissociation of water) is an ionization reaction in pure water or in an aqueous solution, in which a water molecule, H2O, deprotonates (loses the nucleus of one of its hydrogen atoms) to become a hydroxide ion, OH−. The hydrogen nucleus, H+, immediately protonates another water molecule to form a hydronium cation, H3O+. It is an example of autoprotolysis, and exemplifies the amphoteric nature of water.

Ice I<sub>h</sub> Hexagonal crystal form of ordinary ice or frozen water

Ice Ih is the hexagonal crystal form of ordinary ice, or frozen water. Virtually all ice in the biosphere is ice Ih, with the exception only of a small amount of ice Ic that is occasionally present in the upper atmosphere. Ice Ih exhibits many peculiar properties that are relevant to the existence of life and regulation of global climate. For a description of these properties, see Ice, which deals primarily with ice Ih.

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Ice II is a rhombohedral crystalline form of ice with a highly ordered structure. It is formed from ice Ih by compressing it at a temperature of 198 K at 300 MPa or by decompressing ice V. When heated it undergoes transformation to ice III. Ordinary water ice is known as ice Ih,. Different types of ice, from ice II to ice XIX, have been created in the laboratory at different temperatures and pressures. It is thought that the cores of icy moons like Jupiter's Ganymede may be made of ice II.

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Ice IV is a metastable high-pressure phase of ice. It is formed when liquid water is compressed with an immense force.

References

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  12. ↑ Knight, Chris; Singer, Sherwin J. (2007). Kuhs, Werner F. (ed.). Tackling the problem of hydrogen bond order and disorder. Royal Soc. of Chemistry. p. 329. ISBN   9781847557773.{{cite book}}: |work= ignored (help)
  13. 1 2 3 Iitaka, Toshiaki (13 July 2010). "Stability of ferroelectric ice". arXiv: 1007.1792 [cond-mat.mtrl-sci].
  14. ↑ Castro-Neto, A. H.; Pujol, P; Fradkin, Eduardo (21 Jul 2006). "Ice: A strongly correlated proton system". Physical Review Letters. 74 (2): 024302–12. arXiv: cond-mat/0511092 . Bibcode:2006PhRvB..74b4302C. doi:10.1103/PhysRevB.74.024302. S2CID   102581583.
  15. ↑ Fukazawa, Hiroshi; Mae, Shinji; Ikeda, Susumu; Watanabe, Okitsugu (1998). "Proton ordering in Antarctic ice observed by Raman and neutron scattering". Chemical Physics Letters. 294 (6): 554–558. Bibcode:1998CPL...294..554F. doi:10.1016/S0009-2614(98)00908-7.
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  18. ↑ Yen, Fei; Chi, Zhenhua (16 Apr 2015). "Proton ordering dynamics of H2O ice". Physical Chemistry Chemical Physics. 17 (19): 12458–12461. arXiv: 1503.01830 . Bibcode:2015PCCP...1712458Y. doi:10.1039/C5CP01529D. PMID   25912948. S2CID   7736338.
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  20. 1 2 3 4 Arakawa, Masashi; Kagi, Hiroyuki; Fernandez-Baca, Jaime A.; Chakoumakos, Bryan C.; Fukazawa, Hiroshi (17 August 2011). "The existence of memory effect on hydrogen ordering in ice: The effect makes ice attractive". Geophysical Research Letters. 38 (16): n/a. Bibcode:2011GeoRL..3816101A. doi: 10.1029/2011GL048217 .
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  25. ↑ Kawada, Shuji (1 May 1972). "Dielectric Dispersion and Phase Transition of KOH Doped Ice". Journal of the Physical Society of Japan. 32 (5): 1442. Bibcode:1972JPSJ...32.1442K. doi:10.1143/JPSJ.32.1442.
  26. ↑ Tajima, Yoshimitsu; Matsuo, Takasuke; Suga, Hiroshi (1984). "Calorimetric study of phase transition in hexagonal ice doped with alkali hydroxides". Journal of Physics and Chemistry of Solids. 45 (11–12): 1135–1144. Bibcode:1984JPCS...45.1135T. doi:10.1016/0022-3697(84)90008-8.
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  28. ↑ Iedema, M. J.; Dresser, M. J.; Doering, D. L.; Rowland, J. B.; Hess, W. P.; Tsekouras, A. A.; Cowin, J. P. (1 November 1998). "Ferroelectricity in Water Ice". The Journal of Physical Chemistry B. 102 (46): 9203–9214. doi:10.1021/jp982549e. S2CID   97894870.
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  31. 1 2 3 McKinnon, W. B.; Hofmeister, A.M. (August 2005). "Ice XI on Pluto and Charon?". Bulletin of the American Astronomical Society. Division for Planetary Sciences Meeting, American Astronomical Society. 37 (49.02): 732. Bibcode:2005DPS....37.4902M.
  32. ↑ Grossman, Lisa (25 August 2011). "Electric ice a shock to the solar system". New Scientist . Retrieved 7 April 2012.
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  34. ↑ Iedema, M. J.; Dresser, M. J.; Doering, D. L.; Rowland, J. B.; Hess, W. P.; Tsekouras, A. A.; Cowin, J. P. (1998). "Ferroelectricity in Water Ice". The Journal of Physical Chemistry B. American Chemical Society (ACS). 102 (46): 9203–9214. doi:10.1021/jp982549e. ISSN   1520-6106.
  35. ↑ Arakawa, M.; Kagi, H.; Fukazawa, H. (1 October 2009). "Laboratory Measurements of Infrared Absorption Spectra of Hydrogen-Ordered Ice: a Step to the Exploration of Ice XI in Space". The Astrophysical Journal Supplement Series. 184 (2): 361–365. Bibcode:2009ApJS..184..361A. doi: 10.1088/0067-0049/184/2/361 .
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