论文标题

强键固体中的声子 - 音音子相互作用:选择规则和高阶过程

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

论文作者

Ravichandran, Navaneetha K., Broido, David

论文摘要

我们表明,常见使用的声子 - 子声音相互作用的最低阶理论通常无法准确描述Anharmonic的声子衰减速率和导热率($κ$),即使在强键结晶之间也是如此。应用第一原理理论,其中包括最低阶三频率和高阶四频道过程到17个锌Blende半导体,我们发现,最低阶的理论大幅度高估了许多这些材料的测量$κ$,而将四个散射的散射纳入了测量量的一致性。我们已经确定了有关三个频率过程的新选择规则,这些规则有助于解释许多这些失败,这是通过异常弱的非谐声衰变率,该衰减率由最低级的理论与四个phonon过程竞争。我们还表明,含有硼(b),碳(C)或氮(N)原子的锌混合物化合物具有异常弱的四光散射,比不包含B,C或N原子的化合物弱得多。这种新的理解有助于解释几种具有技术重要材料(例如立方硼芳烃,磷化物和碳化硅)的超高$κ$。同时,它不仅使得没有B,C或N原子的材料获得高$κ$的可能性,而且还表明可能有必要在许多以后的研究中包括四个phonon过程。我们的工作给出了固体中非谐波过程的性质的新见解,并证明了高阶声子 - 音纸相互作用在评估材料的热性能中的广泛重要性。

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 lowest-order 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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