Skip to main content
eScholarship
Open Access Publications from the University of California

Predicting finite-temperature properties of crystalline carbon dioxide from first principles with quantitative accuracy.

  • Author(s): Heit, Yonaton N
  • Nanda, Kaushik D
  • Beran, Gregory JO
  • et al.

Published Web Location

http://pubs.rsc.org/en/Content/ArticleLanding/2016/SC/C5SC03014E
No data is associated with this publication.
Abstract

Molecular crystal structures, thermodynamics, and mechanical properties can vary substantially with temperature, and predicting these temperature-dependencies correctly is important for many practical applications in the pharmaceutical industry and other fields. However, most electronic structure predictions of molecular crystal properties neglect temperature and/or thermal expansion, leading to potentially erroneous results. Here, we demonstrate that by combining large basis set second-order Møller-Plesset (MP2) or even coupled cluster singles, doubles, and perturbative triples (CCSD(T)) electronic structure calculations with a quasiharmonic treatment of thermal expansion, experimentally observable properties such as the unit cell volume, heat capacity, enthalpy, entropy, sublimation point and bulk modulus of phase I crystalline carbon dioxide can be predicted in excellent agreement with experiment over a broad range of temperatures. These results point toward a promising future for ab initio prediction of molecular crystal properties at real-world temperatures and pressures.

Many UC-authored scholarly publications are freely available on this site because of the UC's open access policies. Let us know how this access is important for you.

Item not freely available? Link broken?
Report a problem accessing this item