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Title: 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:
 [1];  [1];  [2]; ORCiD logo [1];  [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States). G.W. Woodruff School of Mechanical Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (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. doi: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. doi: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 = {2018},
month = {9}
}

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Figures / Tables:

FIG. 1 FIG. 1: (a) The electron band structure of Ca2N along high symmetry paths in the first Brillouin zone of the conventional hexagonal unit cell. (b) The Brillouin zone of the conventional hexagonal unit cell. (c) The hexagonal unit cell structure with calcium atoms given in green, nitrogen atoms given inmore » red, and a representation of the electron layers given in blue. (d) The phonon dispersion along high symmetry points in the first Brillouin zone of the conventional hexagonal unit cell. (e) The phonon projected density of states.« less

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    Works referencing / citing this record:

    First-principles Modeling of Thermal Transport in Materials: Achievements, Opportunities, and Challenges
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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.