High-pressure polymorphism of to 75 GPa
Abstract
Lead fluoride, PbF2, was investigated experimentally in the laser-heated diamond anvil cell by x-ray diffraction to pressures of 75 GPa at room temperature and to 64.5 GPa and 2430 K, as well as through first-principles density functional theory calculations up to 70 GPa. During room temperature compression, no discontinuous changes in the x-ray diffraction pattern or volume were observed, but the lattice parameters displayed highly anomalous trends between 10-22 GPa with enhanced compressibility along the a direction and reduced or even negative compressibility along b and c. Theoretical calculations of valence electron densities at 22 GPa showed that α-PbF2 underwent a pressure-induced isosymmetric phase transition to a postcotunnite Co2Si structure and also revealed the detailed atomic rearrangements associated with the development of an extra Pb-F bond in the high-pressure phase. Our x-ray results and theoretical calculations are consistent with an isosymmetric phase transition smoothly occurring over 10-22 GPa rather than abruptly as previously suggested. The characteristic values for the cell constants a/c and (a+c)/b, which are used to distinguish among cotunnite-, Co2Si-, and Ni2In-type phases, require modification based on our results. An equation of state fit yields a bulk modulus, K0, of 72(3) GPa for the cotunnite-type, and an ambient-pressuremore »
- Authors:
-
- Princeton Univ., NJ (United States). Dept. of Chemistry
- Princeton Univ., NJ (United States). Dept. of Geosciences
- Princeton Univ., NJ (United States). Dept. of Civil and Environmental Engineering and Andlinger Center for Energy and the Environment
- Argonne National Lab. (ANL) and Univ. of Chicago, Argonne, IL (United States). GeoSoilEnviroCARS
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF)
- OSTI Identifier:
- 1440934
- Alternate Identifier(s):
- OSTI ID: 1260434
- Grant/Contract Number:
- AC02-05CH11231; EAR-1415321; AC02-06CH11357; EAR-1128799; FG02-94ER14466
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 94; Journal Issue: 2; Related Information: © 2016 American Physical Society.; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; pressure effects; solid-solid transformations; density functional theory; x-ray defraction
Citation Formats
Stan, Camelia V., Dutta, Rajkrishna, White, Claire E., Prakapenka, Vitali, and Duffy, Thomas S. High-pressure polymorphism of PbF2 to 75 GPa. United States: N. p., 2016.
Web. doi:10.1103/PhysRevB.94.024104.
Stan, Camelia V., Dutta, Rajkrishna, White, Claire E., Prakapenka, Vitali, & Duffy, Thomas S. High-pressure polymorphism of PbF2 to 75 GPa. United States. https://doi.org/10.1103/PhysRevB.94.024104
Stan, Camelia V., Dutta, Rajkrishna, White, Claire E., Prakapenka, Vitali, and Duffy, Thomas S. Wed .
"High-pressure polymorphism of PbF2 to 75 GPa". United States. https://doi.org/10.1103/PhysRevB.94.024104. https://www.osti.gov/servlets/purl/1440934.
@article{osti_1440934,
title = {High-pressure polymorphism of PbF2 to 75 GPa},
author = {Stan, Camelia V. and Dutta, Rajkrishna and White, Claire E. and Prakapenka, Vitali and Duffy, Thomas S.},
abstractNote = {Lead fluoride, PbF2, was investigated experimentally in the laser-heated diamond anvil cell by x-ray diffraction to pressures of 75 GPa at room temperature and to 64.5 GPa and 2430 K, as well as through first-principles density functional theory calculations up to 70 GPa. During room temperature compression, no discontinuous changes in the x-ray diffraction pattern or volume were observed, but the lattice parameters displayed highly anomalous trends between 10-22 GPa with enhanced compressibility along the a direction and reduced or even negative compressibility along b and c. Theoretical calculations of valence electron densities at 22 GPa showed that α-PbF2 underwent a pressure-induced isosymmetric phase transition to a postcotunnite Co2Si structure and also revealed the detailed atomic rearrangements associated with the development of an extra Pb-F bond in the high-pressure phase. Our x-ray results and theoretical calculations are consistent with an isosymmetric phase transition smoothly occurring over 10-22 GPa rather than abruptly as previously suggested. The characteristic values for the cell constants a/c and (a+c)/b, which are used to distinguish among cotunnite-, Co2Si-, and Ni2In-type phases, require modification based on our results. An equation of state fit yields a bulk modulus, K0, of 72(3) GPa for the cotunnite-type, and an ambient-pressure volume, V0, of 182(2)Å3, and K0=81(4)GPa for the Co2Si-type phase when fixing the pressure derivative of the bulk modulus, K0'=4. Upon heating above 1200 K at pressures at or above 25.9 GPa, PbF2 partially transformed to the hexagonal Ni2In-type phase but wholly or partially reverted back to Co2Si-type phase upon temperature quench. From 43-65 GPa, nearly complete transformation to the Ni2In-type PbF2 was observed at high temperature, but the material partially transformed back to the orthorhombic phase upon temperature quench. Our results show that high-pressure behavior of PbF2 is distinct from that of the alkaline earth fluorides with similar ionic radii. These results also have relevance to understanding the behavior of lanthanide and actinide dioxides, which have been predicted theoretically to exhibit similar isosymmetric transitions at Mbar pressures.},
doi = {10.1103/PhysRevB.94.024104},
journal = {Physical Review B},
number = 2,
volume = 94,
place = {United States},
year = {2016},
month = {7}
}
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