Phonon transport properties of two-dimensional electride Ca2N—A first-principles study
Abstract
We investigate phonon transport in dicalcium nitride (Ca2N), an electride with two-dimensional confined electron layers, using first-principles density functional theory and the phonon Boltzmann transport equation. The in-plane (κ[100]) and out-of-plane (κ[001]) lattice thermal conductivities at 300 K are found to be 11.72 W m-1 K-1 and 2.50 W m-1 K-1, respectively. Spectral analysis of lattice thermal conductivity shows that ~85% of $$κ_{[100]}$$ and $$κ_{[001]}$$ is accumulated by phonons with frequencies less than 5.5 THz and 2.5 THz, respectively. Modal decomposition of lattice thermal conductivity further reveals that the optical phonons contribute to ~68% and ~55% of overall $$κ_{[100]}$$ and $$κ_{[001]}$$, respectively. Phonon dispersion suggests that the large optical phonon contribution is a result of low frequency optical phonons with high group velocities and the lack of phonon bandgap between the acoustic and optical phonon branches. We find that the optical phonons with frequencies below ~5.5 THz have similar three-phonon phase space and scattering rates as acoustic phonons. Comparison of the contributions from emission and absorption processes reveals that the three-phonon phase space and scattering rates of phonons—optical or acoustic—with frequencies below 5.5 THz are largely dominated by absorption processes. We conclude that the large contribution to lattice thermal conductivity by optical phonons is due to the presence of multiple low frequency optical phonon modes with high group velocities and similar phase space and scattering rates as the acoustic phonons. This study provides the frequency and temperature dependent lattice thermal conductivity and insights into phonon transport in Ca2N, both of which have important implications for the development of Ca2N based devices.
- Authors:
-
- Georgia Inst. of Technology, Atlanta, GA (United States). G.W. Woodruff School of Mechanical Engineering
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE
- OSTI Identifier:
- 1543886
- Alternate Identifier(s):
- OSTI ID: 1474771
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Applied Physics Letters
- Additional Journal Information:
- Journal Volume: 113; Journal Issue: 13; Journal ID: ISSN 0003-6951
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Physics
Citation Formats
Barry, Matthew C., Yan, Zhequan, Yoon, Mina, Kalidindi, Surya R., and Kumar, Satish. Phonon transport properties of two-dimensional electride Ca2N—A first-principles study. United States: N. p., 2018.
Web. doi:10.1063/1.5051465.
Barry, Matthew C., Yan, Zhequan, Yoon, Mina, Kalidindi, Surya R., & Kumar, Satish. Phonon transport properties of two-dimensional electride Ca2N—A first-principles study. United States. https://doi.org/10.1063/1.5051465
Barry, Matthew C., Yan, Zhequan, Yoon, Mina, Kalidindi, Surya R., and Kumar, Satish. Fri .
"Phonon transport properties of two-dimensional electride Ca2N—A first-principles study". United States. https://doi.org/10.1063/1.5051465. https://www.osti.gov/servlets/purl/1543886.
@article{osti_1543886,
title = {Phonon transport properties of two-dimensional electride Ca2N—A first-principles study},
author = {Barry, Matthew C. and Yan, Zhequan and Yoon, Mina and Kalidindi, Surya R. and Kumar, Satish},
abstractNote = {We investigate phonon transport in dicalcium nitride (Ca2N), an electride with two-dimensional confined electron layers, using first-principles density functional theory and the phonon Boltzmann transport equation. The in-plane (κ[100]) and out-of-plane (κ[001]) lattice thermal conductivities at 300 K are found to be 11.72 W m-1 K-1 and 2.50 W m-1 K-1, respectively. Spectral analysis of lattice thermal conductivity shows that ~85% of $κ_{[100]}$ and $κ_{[001]}$ is accumulated by phonons with frequencies less than 5.5 THz and 2.5 THz, respectively. Modal decomposition of lattice thermal conductivity further reveals that the optical phonons contribute to ~68% and ~55% of overall $κ_{[100]}$ and $κ_{[001]}$, respectively. Phonon dispersion suggests that the large optical phonon contribution is a result of low frequency optical phonons with high group velocities and the lack of phonon bandgap between the acoustic and optical phonon branches. We find that the optical phonons with frequencies below ~5.5 THz have similar three-phonon phase space and scattering rates as acoustic phonons. Comparison of the contributions from emission and absorption processes reveals that the three-phonon phase space and scattering rates of phonons—optical or acoustic—with frequencies below 5.5 THz are largely dominated by absorption processes. We conclude that the large contribution to lattice thermal conductivity by optical phonons is due to the presence of multiple low frequency optical phonon modes with high group velocities and similar phase space and scattering rates as the acoustic phonons. This study provides the frequency and temperature dependent lattice thermal conductivity and insights into phonon transport in Ca2N, both of which have important implications for the development of Ca2N based devices.},
doi = {10.1063/1.5051465},
journal = {Applied Physics Letters},
number = 13,
volume = 113,
place = {United States},
year = {Fri Sep 28 00:00:00 EDT 2018},
month = {Fri Sep 28 00:00:00 EDT 2018}
}
Web of Science
Figures / Tables:
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