Gimondi, I;
Salvalaglio, M;
(2017)
CO 2 packing polymorphism under pressure: Mechanism and thermodynamics of the I-III polymorphic transition.
The Journal of Chemical Physics
, 147
, Article 114502. 10.1063/1.4993701.
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Abstract
In this work, we describe the thermodynamics and mechanism of CO2 polymorphic transitions under pressure from form I to form III combining standard molecular dynamics, well-tempered metadynamics, and committor analysis. We find that the phase transformation takes place through a concerted rearrangement of CO2 molecules, which unfolds via an anisotropic expansion of the CO2 supercell. Furthermore, at high pressures, we find that defected form I configurations are thermodynamically more stable with respect to form I without structural defects. Our computational approach shows the capability of simultaneously providing an extensive sampling of the configurational space, estimates of the thermodynamic stability, and a suitable description of a complex, collective polymorphic transition mechanism.
| Type: | Article |
|---|---|
| Title: | CO 2 packing polymorphism under pressure: Mechanism and thermodynamics of the I-III polymorphic transition |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1063/1.4993701 |
| Publisher version: | https://doi.org/10.1063/1.4993701 |
| Language: | English |
| Additional information: | This version is the version of record. For information on re-use, please refer to the publisher’s terms and conditions. |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering |
| URI: | https://discovery.ucl.ac.uk/id/eprint/1575799 |
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