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Ab initio structure determination of the low-temperature phase of succinonitrile from laboratory X-ray powder diffraction data—Coping with potential poor powder quality using DFT ab initio methods

Published online by Cambridge University Press:  29 February 2012

P. S. Whitfield ,
Y. Le Page ,
A. Abouimrane  and
I. J. Davidson
P. S. Whitfield
Affiliation:
Institute for Chemical Process and Environmental Technology, National Research Council Canada, 1200 Montreal Road, Ottawa, Ontario K1A 0R6, Canada
Y. Le Page
Affiliation:
Institute for Chemical Process and Environmental Technology, National Research Council Canada, 1200 Montreal Road, Ottawa, Ontario K1A 0R6, Canada
A. Abouimrane
Affiliation:
Institute for Chemical Process and Environmental Technology, National Research Council Canada, 1200 Montreal Road, Ottawa, Ontario K1A 0R6, Canada
I. J. Davidson
Affiliation:
Institute for Chemical Process and Environmental Technology, National Research Council Canada, 1200 Montreal Road, Ottawa, Ontario K1A 0R6, Canada
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Abstract

Without experimental or predicted literature crystal structures for succinonitrile at low temperature, structure solution was attempted from powder diffraction data taken at 173 and 90 K from a solid sample. Its room-temperature plastic-crystal state makes production of a sample with good particle statistics and random orientation almost impossible. Combining constrained models, simulated annealing, and careful application of second-order spherical harmonic corrections nevertheless produced viable-looking structures at 90 and 173 K, yielding two distinct structure models with the same projection down c. VASP optimization of atom coordinates in the experimental cell agreed well with the 90 K model but poorly with the model derived from the 173 K data. The refined 90 K structure changed little on optimization and fitted all datasets from 85 to 225 K. Plots of cell data, torsion angles, and isotropic displacement parameters against temperature suggest possible phase transitions around 100, 120, and 180 K. Cell data at 90 K: monoclinic P21/a, a=9.0851(5) Å, b=8.5617(5) Å, c=5.8343(3) Å, β=79.295(2)°, and Z=4. Succinonitrile has gauche conformation, in agreement with literature spectroscopy data.

Keywords

structure solutionDFT methodssimulated annealingnonambient diffraction

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Type
Technical Articles
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Powder Diffraction , Volume 23 , Issue 4 , December 2008 , pp. 292 - 299
Copyright
Copyright © Cambridge University Press 2008

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