Carbon nitride frameworks and dense crystalline polymorphs
Abstract
Here, we used ab initio random structure searching (AIRSS) to investigate polymorphism in C3N4 carbon nitride as a function of pressure. Our calculations reveal new framework structures, including a particularly stable chiral polymorph of space group P43212 containing mixed sp2 and sp3 bonding, that we have produced experimentally and recovered to ambient conditions. As pressure is increased a sequence of structures with fully sp3-bonded C atoms and three-fold-coordinated N atoms is predicted, culminating in a dense Pnma phase above 250 GPa. Beyond 650 GPa we find that C3N4 becomes unstable to decomposition into diamond and pyrite-structured CN2.
- Authors:
-
- Univ. College London, London (United Kingdom); Univ. of Cambridge, Cambridge (United Kingdom)
- Harvard Univ., Cambridge, MA (United States); Univ. of Nevada, Las Vegas, NV (United States)
- Charles Univ., Prague (Czech Republic); Institute of Organic Chemistry and Biochemistry ASCR, Prague (Czech Republic)
- Cavendish Lab., Cambridge (United Kingdom)
- Univ. College London, London (United Kingdom)
- Publication Date:
- Research Org.:
- Univ. of Nevada, Las Vegas, NV (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1332551
- Grant/Contract Number:
- NA0001982
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 94; Journal Issue: 9; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Pickard, Chris J., Salamat, Ashkan, Bojdys, Michael J., Needs, Richard J., and McMillan, Paul F. Carbon nitride frameworks and dense crystalline polymorphs. United States: N. p., 2016.
Web. doi:10.1103/PhysRevB.94.094104.
Pickard, Chris J., Salamat, Ashkan, Bojdys, Michael J., Needs, Richard J., & McMillan, Paul F. Carbon nitride frameworks and dense crystalline polymorphs. United States. https://doi.org/10.1103/PhysRevB.94.094104
Pickard, Chris J., Salamat, Ashkan, Bojdys, Michael J., Needs, Richard J., and McMillan, Paul F. Thu .
"Carbon nitride frameworks and dense crystalline polymorphs". United States. https://doi.org/10.1103/PhysRevB.94.094104. https://www.osti.gov/servlets/purl/1332551.
@article{osti_1332551,
title = {Carbon nitride frameworks and dense crystalline polymorphs},
author = {Pickard, Chris J. and Salamat, Ashkan and Bojdys, Michael J. and Needs, Richard J. and McMillan, Paul F.},
abstractNote = {Here, we used ab initio random structure searching (AIRSS) to investigate polymorphism in C3N4 carbon nitride as a function of pressure. Our calculations reveal new framework structures, including a particularly stable chiral polymorph of space group P43212 containing mixed sp2 and sp3 bonding, that we have produced experimentally and recovered to ambient conditions. As pressure is increased a sequence of structures with fully sp3-bonded C atoms and three-fold-coordinated N atoms is predicted, culminating in a dense Pnma phase above 250 GPa. Beyond 650 GPa we find that C3N4 becomes unstable to decomposition into diamond and pyrite-structured CN2.},
doi = {10.1103/PhysRevB.94.094104},
journal = {Physical Review B},
number = 9,
volume = 94,
place = {United States},
year = {Thu Sep 08 00:00:00 EDT 2016},
month = {Thu Sep 08 00:00:00 EDT 2016}
}
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Figures / Tables:
FIG. 1: (Color online) Enthalpy per atom for carbon graphite relative to diamond as a function of pressure calculated using fi ve different density functionals (LDA, PBE, PBEsol, PBEG06 and WC).
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