Polymorphism in Br2 clathrate hydrates

The Journal of Physical Chemistry. a
I U GoldschlegerV A Apkarian

Abstract

The structure and composition of bromine clathrate hydrate has been controversial for more than 170 years due to the large variation of its observed stoichiometries. Several different crystal structures were proposed before 1997 when Udachin et al. (Udachin, K. A.; Enright, G. D.; Ratcliffe, C. I.; Ripmeester, J. A. J. Am. Chem. Soc. 1997, 119, 11481) concluded that Br2 forms only the tetragonal structure (TS-I). We show polymorphism in Br2 clathrate hydrates by identifying two distinct crystal structures through optical microscopy and resonant Raman spectroscopy on single crystals. After growing TS-I crystals from a liquid bromine-water solution, upon dropping the temperature slightly below -7 degrees C, new crystals of cubic morphology form. The new crystals, which have a limited thermal stability range, are assigned to the CS-II structure. The two structures are clearly distinguished by the resonant Raman spectra of the enclathrated Br2, which show long overtone progressions and allow the extraction of accurate vibrational parameters: omega(e) = 321.2 +/- 0.1 cm(-1) and omega(e)x(e) = 0.82 +/- 0.05 cm(-1) in TS-I and omega(e) = 317.5 +/- 0.1 cm(-1) and omega(e)x(e) = 0.70 +/- 0.1 cm(-1) in CS-II. On the basis of structural a...Continue Reading

References

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Citations

Oct 23, 2013·Journal of Colloid and Interface Science·O SalakoJ W Lee
Feb 3, 2011·The Journal of Physical Chemistry. a·Ricardo Franklin-MergarejoKenneth C Janda
Aug 25, 2011·The Journal of Chemical Physics·Liam C JacobsonValeria Molinero
Jul 26, 2013·The Journal of Chemical Physics·I U GoldschlegerV Ara Apkarian
May 10, 2011·The Journal of Chemical Physics·Edward T BraniganV A Apkarian
Feb 8, 2016·The Journal of Chemical Physics·Ricardo Franklin-MergarejoV Ara Apkarian
Feb 2, 2016·The Journal of Chemical Physics·Hana DureckovaSaman Alavi
Nov 19, 2015·Journal of Chemical Theory and Computation·Octavio RonceroRamón Hernández-Lamoneda
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May 31, 2011·The Journal of Physical Chemistry. B·Masakazu Matsumoto, Hideki Tanaka
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Nov 3, 2016·The Journal of Chemical Physics·David Ochoa-ResendizRamón Hernández-Lamoneda
Dec 9, 2008·Physical Chemistry Chemical Physics : PCCP·I U GoldschlegerV A Apkarian
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