Proton disorder in dehydrated hemimorphite - IR spectroscopy and X-ray structure refinement at low and ambient temperatures

Author(s)
Eugen Libowitzky, George R. Rossman, Thomas Armbruster, Thomas Kohler
Abstract

Polarized IR absorption spectra of dehydrated hemimorphite single-crystals [Zn4Si2O7(OH)2] were recorded between 82 and 373 K. The crystal structure, including the proton positions, was refined in space group Imm2 from single-crystal x-ray data measured at 110 and 298 K. Both methods, as well as electrostatic and crystal chem. considerations, show that the protons of the hydroxide groups are disordered in the structural channels. One proton is located at the line between two O3 atoms (O3×××O3' = 2.99-3.02 .ANG.) thus building up a weak H bond. The corresponding O-H stretching band occurs at .apprx.3530 cm-1 and is polarized parallel to a. Due to proton-proton repulsion, the O-H vector of the other H atom deviates from the O3×××O3' line. As a consequence, the corresponding IR stretching vibration is obsd. at .apprx.3600 cm-1 and components of this band occur parallel to a and c. The disorder is also reflected by the large anisotropic displacement parameter U33 of the O3 atom. To test for a possible low-temp. phase transition (similar to that in natural hemimorphite), birefringence values were detd. in (010) and (001) sections between 83 and 373 K. However, the smooth curves do not indicate a transition. This is explained by the lack of an addnl. proton acceptor (O5 of the water mol. in hemimorphite) in the dehydrated phase.

Organisation(s)
Department of Mineralogy and Crystallography
External organisation(s)
California Institute of Technology (Caltech), Universität Bern
Journal
European Journal of Mineralogy: an international journal of mineralogy, geochemistry and related sciences
Volume
9
Pages
803-810
No. of pages
18
ISSN
0935-1221
Publication date
1997
Peer reviewed
Yes
Austrian Fields of Science 2012
105113 Crystallography, 105116 Mineralogy, 104026 Spectroscopy
Portal url
https://ucrisportal.univie.ac.at/en/publications/proton-disorder-in-dehydrated-hemimorphite--ir-spectroscopy-and-xray-structure-refinement-at-low-and-ambient-temperatures(21e40bfc-47e6-4a06-b13c-69d794228de4).html