Lattice Thermal Conductivity of Polyethylene Molecular Crystals from First-Principles Including Nuclear Quantum Effects
Abstract
Molecular crystals such as polyethylene are of intense interest as flexible thermal conductors, yet their intrinsic upper limits of thermal conductivity remain unknown. Here, we report a study of the vibrational properties and lattice thermal conductivity of a polyethylene molecular crystal using an ab initio approach that rigorously incorporates nuclear quantum motion and finite temperature effects. We obtain a thermal conductivity along the chain direction of around 160 W m^(-1) K^(-1) at room temperature, providing a firm upper bound for the thermal conductivity of this molecular crystal. Furthermore, we show that the inclusion of quantum nuclear effects significantly impacts the thermal conductivity by altering the phase space for three-phonon scattering. Our computational approach paves the way for ab initio studies and computational material discovery of molecular solids free of any adjustable parameters.
Additional Information
© 2017 American Physical Society. Received 6 April 2017; revised manuscript received 14 June 2017; published 31 October 2017. N. S. and A. J. M. acknowledge the support of the DARPA MATRIX program under Grant No. HR0011-15-2-0039 and an ONR Young Investigator Award under Grant No. N00014-15-1-2688. O. H. acknowledges the support from the Swedish Research Council (VR) Program No. 637-2013-7296. This work used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation Grant No. ACI-1053575 and the Swedish National Infrastructure for Computing (SNIC) at PDC center (High Performance Computing at the KTH Royal Institute of Technology) and National Supercomputer Center (NSC, Linköping University). N. S. and O. H. contributed equally to this work.Attached Files
Published - PhysRevLett.119.185901.pdf
Files
Name | Size | Download all |
---|---|---|
md5:bf0d3325bfb5b4458c8ed3ef7354a8c1
|
652.7 kB | Preview Download |
Additional details
- Eprint ID
- 82810
- Resolver ID
- CaltechAUTHORS:20171031-135346052
- Defense Advanced Research Projects Agency (DARPA)
- HR0011-15-2-0039
- Office of Naval Research (ONR)
- N00014-15-1-2688
- Swedish Research Council
- 637-2013-7296
- NSF
- ACI-1053575
- KTH Royal Institute of Technology
- Linköping University
- Created
-
2017-10-31Created from EPrint's datestamp field
- Updated
-
2021-11-15Created from EPrint's last_modified field