Electron and phonon interactions and transport in the ultrahigh-temperature ceramic ZrC

Mellan, Thomas A.; Aziz, Alex; Xia, Yi; Grau‐Crespo, Ricardo; Duff, Andrew Ian

doi:10.1103/physrevb.99.094310

Cited by 13 publications

(9 citation statements)

References 55 publications

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“…The implications of this finding are discussed below. Interestingly, recent calculations of thermal transport in ZrC [21], a metal with rock salt structure, also show unusually weak four-phonon scattering rates and correspondingly small reductions in the phonon-phonon limited κ, consistent with our findings for the zinc blende BCN compounds.…”

Section: Four-phonon Scattering and Its Weakness In Compounds With Bo...supporting

confidence: 91%

“…Inclusion of four-phonon interactions in ab initio anharmonic decay rates and transport calculations is computationally challenging, and such calculations are currently performed by only a small number of groups [12][13][14][15][16][17][18][19][20][21]. Recent work has shown that for strongly anharmonic materials, it is essential to include four-phonon processes [14][15][16].…”

Section: Discussionmentioning

confidence: 99%

“…While this lowest-order theory has been generally assumed to adequately describe anharmonic properties of crystals, ab initio descriptions of higher-order four-phonon interactions are now becoming possible [12][13][14][15][16][17][18][19][20][21]. One might expect higher-order phonon-phonon interactions to be important in strongly anharmonic * navaneeth@iisc.ac.in materials, i.e., those with weak chemical bonds.…”

Section: Introductionmentioning

confidence: 99%

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Phonon-Phonon Interactions in Strongly Bonded Solids: Selection Rules and Higher-Order Processes

Ravichandran,

Broido

2020

Preprint

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We show that the commonly used lowest-order theory of phonon-phonon interactions frequently fails to accurately describe the anharmonic phonon decay rates and thermal conductivity (κ), even among strongly bonded crystals. Applying a first principles theory that includes both the lowestorder three-phonon and the higher-order four-phonon processes to seventeen zinc blende semiconductors, we find that the lowest-order theory drastically overestimates the measured κ for many of these materials, while inclusion of four-phonon scattering gives significantly improved agreement with measurements. We have identified new selection rules on three-phonon processes that help explain many of these failures in terms of anomalously weak anharmonic phonon decay rates predicted by the lowest-order theory competing with four-phonon processes. We also show that zinc blende compounds containing boron (B), carbon (C) or nitrogen (N) atoms have exceptionally weak four-phonon scattering, much weaker than in compounds that do not contain B, C or N atoms. This new understanding helps explain the ultrahigh κ in several technologically important materials like cubic boron arsenide, boron phosphide and silicon carbide. At the same time, it not only makes the possibility of achieving high κ in materials without B, C or N atoms unlikely, but it also suggests that it may be necessary to include four-phonon processes in many future studies. Our work gives new insights into the nature of anharmonic processes in solids and demonstrates the broad importance of higher-order phonon-phonon interactions in assessing the thermal properties of materials.

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Section: Four-phonon Scattering and Its Weakness In Compounds With Bo...supporting

confidence: 91%

Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Phonon-Phonon Interactions in Strongly Bonded Solids: Selection Rules and Higher-Order Processes

Ravichandran,

Broido

2020

Preprint

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“…Also, the thermal conductivity increases with increasing temperature. The thermal conductivity of ZrC over a wide temperature range was predicted using a single‐mode relaxation time approximation to calculate the phonon thermal conductivity, and a semi‐classical method was employed to calculate the electron thermal conductivity 20 . The total thermal conductivity was predicted to be affected by grain size, that is, larger grain size favored higher thermal conductivity.…”

Section: Introductionmentioning

confidence: 99%

First‐principles study of the thermal properties of Zr₂C and Zr₂CO

et al. 2022

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First‐principles calculations of lattice thermal conductivities and thermodynamic properties of Zr2C and Zr2CO were performed using the quasi‐harmonic approximation. Oxygen in the lattice gives Zr2CO higher bonding strength than Zr2C. Thus, the mechanical properties of Zr2C are enhanced when the vacancies in its crystal structure are filled with oxygen. Among the critical parameters that determine the lattice thermal conductivity, Zr2C has significantly higher Grüneisen parameters, thus Zr2C has lower lattice thermal conductivity than Zr2CO. In addition, Zr2CO has a higher heat capacity and thermal expansion coefficient than Zr2C at most temperatures. These results indicate that the addition of oxygen has increased the stiffness and thermal conductivity of zirconium carbide that contains a large fraction of carbon vacancies due to the filling of vacancies in the Zr2C lattice and the formation of Zr–O bonds.

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“…Ultra-high-temperature ceramics (UHTCs) make up a class of materials with high melting points of >3000 °C, , which find applications as surface coating materials for use in hypersonic flight, rocket propulsion, and space shuttles, where the friction between aerocrafts and the Earth’s atmosphere produces a tremendous amount of heat. − Many transition-metal (TM) light-element compounds, such as ZrB 2 , HfB 2 , ZrC, and HfN, are good UHTC materials. − Among TM borides, − ZrB 2 has attracted a great deal of interest because of its superior ability to resist oxidation and its desirable mechanical and thermal properties. − ZrB 2 has a high melting temperature of 3246 K, which is particularly important for its use as an UHTC material in extreme thermal environments.…”

mentioning

confidence: 99%

Indentation Strengths of Zirconium Diboride: Intrinsic versus Extrinsic Mechanisms

Chen

2021

J. Phys. Chem. Lett.

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Zirconium diboride (ZrB 2 ) is an important ultrahigh-temperature ceramic, which exhibits outstanding mechanical properties and is widely used in extreme environments. Extensive experimental studies, however, have found that synthesized ZrB 2 specimens show widely scattered indentation hardness values ranging from 8.7 to 26 GPa. We have performed comprehensive stress−strain calculations of ZrB 2 to explore its structural and stress responses and found that ZrB 2 possesses an intrinsic indentation strength of 32.7 GPa, which is on par with those of other transition-metal borides that exhibit higher indentation hardness values of ∼30 GPa. This result suggests that large variations in measured hardness are driven by extrinsic factors, and an analysis of available experimental data indicates that the quality of the crystallinity of specimens holds the key to realizing improved hardness corresponding to the predicted intrinsic indentation strength. These findings offer insights into the origin of the previously reported lower hardness values of ZrB 2 and raise the prospects of achieving superior strengths in well-crystallized ZrB 2 that approach or match those of other ultrahard transition-metal compounds.

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Electron and phonon interactions and transport in the ultrahigh-temperature ceramic ZrC

Cited by 13 publications

References 55 publications

Phonon-Phonon Interactions in Strongly Bonded Solids: Selection Rules and Higher-Order Processes

Phonon-Phonon Interactions in Strongly Bonded Solids: Selection Rules and Higher-Order Processes

First‐principles study of the thermal properties of Zr₂C and Zr₂CO

Indentation Strengths of Zirconium Diboride: Intrinsic versus Extrinsic Mechanisms

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Electron and phonon interactions and transport in the ultrahigh-temperature ceramic ZrC

Cited by 13 publications

References 55 publications

Phonon-Phonon Interactions in Strongly Bonded Solids: Selection Rules and Higher-Order Processes

Phonon-Phonon Interactions in Strongly Bonded Solids: Selection Rules and Higher-Order Processes

First‐principles study of the thermal properties of Zr2C and Zr2CO

Indentation Strengths of Zirconium Diboride: Intrinsic versus Extrinsic Mechanisms

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First‐principles study of the thermal properties of Zr₂C and Zr₂CO