Ab initio phonon point defect scattering and thermal transport in graphene
Abstract
Here, we study the scattering of phonons from point defects and their effect on lattice thermal conductivity κ using a parameter-free ab initio Green's function methodology. Specifically, we focus on the scattering of phonons by boron (B), nitrogen (N), and phosphorus substitutions as well as single- and double-carbon vacancies in graphene. We show that changes of the atomic structure and harmonic interatomic force constants locally near defects govern the strength and frequency trends of the scattering of out-of-plane acoustic (ZA) phonons, the dominant heat carriers in graphene. ZA scattering rates due to N substitutions are nearly an order of magnitude smaller than those for B defects despite having similar mass perturbations. Furthermore, ZA phonon scattering rates from N defects decrease with increasing frequency in the lower-frequency spectrum in stark contrast to expected trends from simple models. ZA phonon-vacancy scattering rates are found to have a significantly softer frequency dependence (~ω0) in graphene than typically employed in phenomenological models. The rigorous Green's function calculations demonstrate that typical mass-defect models do not adequately describe ZA phonon-defect scattering rates. Our ab initio calculations capture well the trend of κ vs vacancy density from experiments, though not the magnitudes. In conclusion, this work elucidatesmore »
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1422989
- Alternate Identifier(s):
- OSTI ID: 1415670
- Grant/Contract Number:
- AC05-00OR22725; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 97; Journal Issue: 1; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Polanco, Carlos A., and Lindsay, Lucas R. Ab initio phonon point defect scattering and thermal transport in graphene. United States: N. p., 2018.
Web. doi:10.1103/PhysRevB.97.014303.
Polanco, Carlos A., & Lindsay, Lucas R. Ab initio phonon point defect scattering and thermal transport in graphene. United States. https://doi.org/10.1103/PhysRevB.97.014303
Polanco, Carlos A., and Lindsay, Lucas R. Thu .
"Ab initio phonon point defect scattering and thermal transport in graphene". United States. https://doi.org/10.1103/PhysRevB.97.014303. https://www.osti.gov/servlets/purl/1422989.
@article{osti_1422989,
title = {Ab initio phonon point defect scattering and thermal transport in graphene},
author = {Polanco, Carlos A. and Lindsay, Lucas R.},
abstractNote = {Here, we study the scattering of phonons from point defects and their effect on lattice thermal conductivity κ using a parameter-free ab initio Green's function methodology. Specifically, we focus on the scattering of phonons by boron (B), nitrogen (N), and phosphorus substitutions as well as single- and double-carbon vacancies in graphene. We show that changes of the atomic structure and harmonic interatomic force constants locally near defects govern the strength and frequency trends of the scattering of out-of-plane acoustic (ZA) phonons, the dominant heat carriers in graphene. ZA scattering rates due to N substitutions are nearly an order of magnitude smaller than those for B defects despite having similar mass perturbations. Furthermore, ZA phonon scattering rates from N defects decrease with increasing frequency in the lower-frequency spectrum in stark contrast to expected trends from simple models. ZA phonon-vacancy scattering rates are found to have a significantly softer frequency dependence (~ω0) in graphene than typically employed in phenomenological models. The rigorous Green's function calculations demonstrate that typical mass-defect models do not adequately describe ZA phonon-defect scattering rates. Our ab initio calculations capture well the trend of κ vs vacancy density from experiments, though not the magnitudes. In conclusion, this work elucidates important insights into phonon-defect scattering and thermal transport in graphene, and demonstrates the applicability of first-principles methods toward describing these properties in imperfect materials.},
doi = {10.1103/PhysRevB.97.014303},
journal = {Physical Review B},
number = 1,
volume = 97,
place = {United States},
year = {Thu Jan 04 00:00:00 EST 2018},
month = {Thu Jan 04 00:00:00 EST 2018}
}
Web of Science
Works referenced in this record:
Intrinsic lattice thermal conductivity of semiconductors from first principles
journal, December 2007
- Broido, D. A.; Malorny, M.; Birner, G.
- Applied Physics Letters, Vol. 91, Issue 23
Phonon Dispersion in Graphite
journal, February 2004
- Maultzsch, J.; Reich, S.; Thomsen, C.
- Physical Review Letters, Vol. 92, Issue 7
Effects of functional group mass variance on vibrational properties and thermal transport in graphene
journal, March 2017
- Lindsay, L.; Kuang, Y.
- Physical Review B, Vol. 95, Issue 12
Light non-metallic atom (B, N, O and F)-doped graphene: a first-principles study
journal, November 2010
- Wu, M.; Cao, C.; Jiang, J. Z.
- Nanotechnology, Vol. 21, Issue 50
Quantifying Defects in Graphene via Raman Spectroscopy at Different Excitation Energies
journal, July 2011
- Cançado, L. G.; Jorio, A.; Ferreira, E. H. Martins
- Nano Letters, Vol. 11, Issue 8, p. 3190-3196
Heat transport in silicon from first-principles calculations
journal, August 2011
- Esfarjani, Keivan; Chen, Gang; Stokes, Harold T.
- Physical Review B, Vol. 84, Issue 8
Phonon-isotope scattering and thermal conductivity in materials with a large isotope effect: A first-principles study
journal, October 2013
- Lindsay, L.; Broido, D. A.; Reinecke, T. L.
- Physical Review B, Vol. 88, Issue 14
Role of light and heavy embedded nanoparticles on the thermal conductivity of SiGe alloys
journal, September 2011
- Kundu, A.; Mingo, N.; Broido, D. A.
- Physical Review B, Vol. 84, Issue 12
Phonon dispersion of graphite by inelastic x-ray scattering
journal, July 2007
- Mohr, M.; Maultzsch, J.; Dobardžić, E.
- Physical Review B, Vol. 76, Issue 3
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009
- Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
- Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
Visualizing Individual Nitrogen Dopants in Monolayer Graphene
journal, August 2011
- Zhao, L.; He, R.; Rim, K. T.
- Science, Vol. 333, Issue 6045
Thermal properties of graphene and nanostructured carbon materials
journal, August 2011
- Balandin, Alexander A.
- Nature Materials, Vol. 10, Issue 8, p. 569-581
Graphene: Status and Prospects
journal, June 2009
- Geim, A. K.
- Science, Vol. 324, Issue 5934, p. 1530-1534
Influence of Polymeric Residue on the Thermal Conductivity of Suspended Bilayer Graphene
journal, March 2011
- Pettes, Michael Thompson; Jo, Insun; Yao, Zhen
- Nano Letters, Vol. 11, Issue 3, p. 1195-1200
Ab initio study of the effect of vacancies on the thermal conductivity of boron arsenide
journal, July 2016
- Protik, Nakib Haider; Carrete, Jesús; Katcho, Nebil A.
- Physical Review B, Vol. 94, Issue 4
Gas adsorption on graphene doped with B, N, Al, and S: A theoretical study
journal, December 2009
- Dai, Jiayu; Yuan, Jianmin; Giannozzi, Paolo
- Applied Physics Letters, Vol. 95, Issue 23
Thermal Transport in Suspended and Supported Monolayer Graphene Grown by Chemical Vapor Deposition
journal, May 2010
- Cai, Weiwei; Moore, Arden L.; Zhu, Yanwu
- Nano Letters, Vol. 10, Issue 5, p. 1645-1651
Reliability of Raman measurements of thermal conductivity of single-layer graphene due to selective electron-phonon coupling: A first-principles study
journal, March 2016
- Vallabhaneni, Ajit K.; Singh, Dhruv; Bao, Hua
- Physical Review B, Vol. 93, Issue 12
Thermal conductivity of isotopically modified graphene
journal, January 2012
- Chen, Shanshan; Wu, Qingzhi; Mishra, Columbia
- Nature Materials, Vol. 11, Issue 3
Synthesis, Structure, and Properties of Boron- and Nitrogen-Doped Graphene
journal, August 2009
- Panchakarla, L. S.; Subrahmanyam, K. S.; Saha, S. K.
- Advanced Materials
Extremely high thermal conductivity of graphene: Prospects for thermal management applications in nanoelectronic circuits
journal, April 2008
- Ghosh, S.; Calizo, I.; Teweldebrhan, D.
- Applied Physics Letters, Vol. 92, Issue 15, Article No. 151911
Role of Surface-Segregation-Driven Intermixing on the Thermal Transport through Planar Superlattices
journal, September 2013
- Chen, Peixuan; Katcho, N. A.; Feser, J. P.
- Physical Review Letters, Vol. 111, Issue 11
First-Principles Study of Nitrogen-, Boron-Doped Graphene and Co-Doped Graphene as the Potential Catalysts in Nonaqueous Li–O 2 Batteries
journal, March 2016
- Jiang, H. R.; Zhao, T. S.; Shi, L.
- The Journal of Physical Chemistry C, Vol. 120, Issue 12
Ab initio theory of the lattice thermal conductivity in diamond
journal, September 2009
- Ward, A.; Broido, D. A.; Stewart, Derek A.
- Physical Review B, Vol. 80, Issue 12
Phonon transport in nanowires coated with an amorphous material: An atomistic Green’s function approach
journal, December 2003
- Mingo, N.; Yang, Liu
- Physical Review B, Vol. 68, Issue 24
Thermal conductivity of suspended pristine graphene measured by Raman spectroscopy
journal, February 2011
- Lee, Jae-Ung; Yoon, Duhee; Kim, Hakseong
- Physical Review B, Vol. 83, Issue 8
Phonons and thermal transport in graphene and graphene-based materials
journal, January 2017
- Nika, Denis L.; Balandin, Alexander A.
- Reports on Progress in Physics, Vol. 80, Issue 3
Beyond the isotropic-model approximation in the theory of thermal conductivity
journal, April 1996
- Omini, M.; Sparavigna, A.
- Physical Review B, Vol. 53, Issue 14
Structural Defects in Graphene
journal, November 2010
- Banhart, Florian; Kotakoski, Jani; Krasheninnikov, Arkady V.
- ACS Nano, Vol. 5, Issue 1
Isotope scattering of dispersive phonons in Ge
journal, January 1983
- Tamura, Shin-ichiro
- Physical Review B, Vol. 27, Issue 2
Effect of nitrogen and vacancy defects on the thermal conductivity of diamond: An ab initio Green's function approach
journal, September 2014
- Katcho, N. A.; Carrete, J.; Li, Wu
- Physical Review B, Vol. 90, Issue 9
Quantum thermal transport in nanostructures
journal, April 2008
- Wang, J. -S.; Wang, J.; Lü, J. T.
- The European Physical Journal B, Vol. 62, Issue 4
Ab initio study of the interactions between boron and nitrogen dopants in graphene
journal, August 2012
- Al-Aqtash, Nabil; Al-Tarawneh, Khaldoun M.; Tawalbeh, Tarek
- Journal of Applied Physics, Vol. 112, Issue 3
Thermal and thermoelectric transport measurements of an individual boron arsenide microstructure
journal, May 2016
- Kim, Jaehyun; Evans, Daniel A.; Sellan, Daniel P.
- Applied Physics Letters, Vol. 108, Issue 20
The Scattering of Low-Frequency Lattice Waves by Static Imperfections
journal, December 1955
- Klemens, P. G.
- Proceedings of the Physical Society. Section A, Vol. 68, Issue 12
Thermal Conductivity of Graphene in Corbino Membrane Geometry
journal, March 2010
- Faugeras, Clement; Faugeras, Blaise; Orlita, Milan
- ACS Nano, Vol. 4, Issue 4
Superior Thermal Conductivity of Single-Layer Graphene
journal, March 2008
- Balandin, Alexander A.; Ghosh, Suchismita; Bao, Wenzhong
- Nano Letters, Vol. 8, Issue 3, p. 902-907
Scattering of phonons by vacancies
journal, November 1987
- Ratsifaritana, C. A.; Klemens, P. G.
- International Journal of Thermophysics, Vol. 8, Issue 6
Effect of grain boundaries on thermal transport in graphene
journal, January 2013
- Serov, Andrey Y.; Ong, Zhun-Yong; Pop, Eric
- Applied Physics Letters, Vol. 102, Issue 3
Cluster scattering effects on phonon conduction in graphene
journal, January 2010
- Mingo, Natalio; Esfarjani, K.; Broido, D. A.
- Physical Review B, Vol. 81, Issue 4
Role of graphene defects in corrosion of graphene-coated Cu(111) surface
journal, March 2013
- Wlasny, I.; Dabrowski, P.; Rogala, M.
- Applied Physics Letters, Vol. 102, Issue 11
First-Principles Determination of Ultrahigh Thermal Conductivity of Boron Arsenide: A Competitor for Diamond?
journal, July 2013
- Lindsay, L.; Broido, D. A.; Reinecke, T. L.
- Physical Review Letters, Vol. 111, Issue 2, Article No. 025901
Probing the Nature of Defects in Graphene by Raman Spectroscopy
journal, July 2012
- Eckmann, Axel; Felten, Alexandre; Mishchenko, Artem
- Nano Letters, Vol. 12, Issue 8
Raman Measurements of Thermal Transport in Suspended Monolayer Graphene of Variable Sizes in Vacuum and Gaseous Environments
journal, December 2010
- Chen, Shanshan; Moore, Arden L.; Cai, Weiwei
- ACS Nano, Vol. 5, Issue 1
Hydrodynamic phonon transport in suspended graphene
journal, February 2015
- Lee, Sangyeop; Broido, David; Esfarjani, Keivan
- Nature Communications, Vol. 6, Issue 1
The rise of graphene
journal, March 2007
- Geim, A. K.; Novoselov, K. S.
- Nature Materials, Vol. 6, Issue 3, p. 183-191
Experimental study of the proposed super-thermal-conductor: BAs
journal, February 2015
- Lv, Bing; Lan, Yucheng; Wang, Xiqu
- Applied Physics Letters, Vol. 106, Issue 7
Theory of the lattice thermal conductivity in bulk and films of GaN
journal, May 2010
- AlShaikhi, A.; Barman, Saswati; Srivastava, G. P.
- Physical Review B, Vol. 81, Issue 19
Defect-like Structures of Graphene on Copper Foils for Strain Relief Investigated by High-Resolution Scanning Tunneling Microscopy
journal, April 2011
- Zhang, Yanfeng; Gao, Teng; Gao, Yabo
- ACS Nano, Vol. 5, Issue 5
Self-interaction correction to density-functional approximations for many-electron systems
journal, May 1981
- Perdew, J. P.; Zunger, Alex
- Physical Review B, Vol. 23, Issue 10, p. 5048-5079
First Principles Peierls-Boltzmann Phonon Thermal Transport: A Topical Review
journal, April 2016
- Lindsay, Lucas
- Nanoscale and Microscale Thermophysical Engineering, Vol. 20, Issue 2
Ab initio variational approach for evaluating lattice thermal conductivity
journal, July 2013
- Fugallo, Giorgia; Lazzeri, Michele; Paulatto, Lorenzo
- Physical Review B, Vol. 88, Issue 4
Ab initio phonon scattering by dislocations
journal, June 2017
- Wang, Tao; Carrete, Jesús; van Roekeghem, Ambroise
- Physical Review B, Vol. 95, Issue 24
Phonon thermal transport in strained and unstrained graphene from first principles
journal, April 2014
- Lindsay, L.; Li, Wu; Carrete, Jesús
- Physical Review B, Vol. 89, Issue 15
Phonon hydrodynamics in two-dimensional materials
journal, March 2015
- Cepellotti, Andrea; Fugallo, Giorgia; Paulatto, Lorenzo
- Nature Communications, Vol. 6, Issue 1
Flexural phonons and thermal transport in graphene
journal, September 2010
- Lindsay, L.; Broido, D. A.; Mingo, Natalio
- Physical Review B, Vol. 82, Issue 11
The rise of graphene
book, August 2009
- Rodgers, Peter; Geim, A. K.; Novoselov, K. S.
- Nanoscience and Technology: A Collection of Reviews from Nature Journals, p. 11-19
Quantifying defects in graphene via Raman spectroscopy at different excitation energies.
text, January 2011
- Cançado, Lg; Jorio, A.; Ferreira, EH Martins
- Apollo - University of Cambridge Repository
Ab initio theory of the lattice thermal conductivity in diamond
text, January 2009
- Ward, Alister; Broido, David; Stewart, Derek A.
- Universität Regensburg
Heat transport in silicon from first principles calculations
text, January 2011
- Esfarjani, Keivan; Chen, Gang; Stokes, Harold T.
- arXiv
Visualizing Individual Nitrogen Dopants in Monolayer Graphene
text, January 2011
- Zhao, Liuyan; He, Rui; Rim, Kwang Taeg
- arXiv
Probing the Nature of Defects in Graphene by Raman Spectroscopy
text, January 2012
- Eckmann, Axel; Felten, Alexandre; Mishchenko, Artem
- arXiv
Phonons and Thermal Transport in Graphene and Graphene-Based Materials
text, January 2016
- Nika, Denis L.; Balandin, Alexander A.
- arXiv
Works referencing / citing this record:
Delocalized Nonlinear Vibrational Modes in Graphene: Second Harmonic Generation and Negative Pressure
journal, December 2018
- Korznikova, Elena A.; Shcherbinin, Stepan A.; Ryabov, Denis S.
- physica status solidi (b), Vol. 256, Issue 1
First-principles Modeling of Thermal Transport in Materials: Achievements, Opportunities, and Challenges
journal, December 2019
- Ma, Tengfei; Chakraborty, Pranay; Guo, Xixi
- International Journal of Thermophysics, Vol. 41, Issue 1
Dislocation-induced thermal transport anisotropy in single-crystal group-III nitride films
journal, December 2018
- Sun, Bo; Haunschild, Georg; Polanco, Carlos
- Nature Materials, Vol. 18, Issue 2
Thermal conductivity of two-dimensional BC 3 : a comparative study with two-dimensional C 3 N
journal, January 2019
- Song, Jieren; Xu, Zhonghai; He, Xiaodong
- Physical Chemistry Chemical Physics, Vol. 21, Issue 24
Enhanced n-doping of epitaxial graphene on SiC by bismuth
journal, July 2018
- Hu, Tingwei; Fang, Qinglong; Zhang, Xiaohe
- Applied Physics Letters, Vol. 113, Issue 1
Enhancement of thermoelectric figure-of-merit of graphene upon BN-doping and sample length reduction
journal, September 2018
- D’Souza, Ransell; Mukherjee, Sugata
- Journal of Applied Physics, Vol. 124, Issue 12
Phonon interaction with ripples and defects in thin layered molybdenum disulfide
journal, June 2019
- Smith, Brandon; Lindsay, Lucas; Kim, Jaehyun
- Applied Physics Letters, Vol. 114, Issue 22
Perspective on ab initio phonon thermal transport
journal, August 2019
- Lindsay, Lucas; Katre, Ankita; Cepellotti, Andrea
- Journal of Applied Physics, Vol. 126, Issue 5
Molecular Dynamics Study on the Reverse Osmosis Using Multilayer Porous Graphene Membranes
journal, October 2018
- Zhang, Zhongqiang; Zhang, Fujian; Liu, Zhen
- Nanomaterials, Vol. 8, Issue 10
Dislocation-induced thermal transport anisotropy in single-crystal group-III nitride films
text, January 2018
- Sun, Bo; Haunschild, Georg; Polanco, Carlos
- arXiv
Enhancement of thermoelectric figure-of-merit of Graphene upon BN-doping and sample length reduction
text, January 2018
- D'Souza, Ransell; Mukherjee, Sugata
- arXiv