Department of Materials Science and Engineering , Stanford University , Stanford , California 94305 , United States.
Department of Mechanical Engineering , Stanford University , Stanford , California 94305 , United States.
Nano Lett. 2018 Jun 13;18(6):3466-3472. doi: 10.1021/acs.nanolett.8b00534. Epub 2018 Apr 13.
Understanding the impact of lattice imperfections on nanoscale thermal transport is crucial for diverse applications ranging from thermal management to energy conversion. Grain boundaries (GBs) are ubiquitous defects in polycrystalline materials, which scatter phonons and reduce thermal conductivity (κ). Historically, their impact on heat conduction has been studied indirectly through spatially averaged measurements, that provide little information about phonon transport near a single GB. Here, using spatially resolved time-domain thermoreflectance (TDTR) measurements in combination with electron backscatter diffraction (EBSD), we make localized measurements of κ within few μm of individual GBs in boron-doped polycrystalline diamond. We observe strongly suppressed thermal transport near GBs, a reduction in κ from ∼1000 W m K at the center of large grains to ∼400 W m K in the immediate vicinity of GBs. Furthermore, we show that this reduction in κ is measured up to ∼10 μm away from a GB. A theoretical model is proposed that captures the local reduction in phonon mean-free-paths due to strongly diffuse phonon scattering at the disordered grain boundaries. Our results provide a new framework for understanding phonon-defect interactions in nanomaterials, with implications for the use of high-κ polycrystalline materials as heat sinks in electronics thermal management.
理解晶格缺陷对纳米尺度热输运的影响对于从热管理到能量转换的各种应用至关重要。晶界(GB)是多晶材料中普遍存在的缺陷,它们会散射声子并降低热导率(κ)。历史上,通过空间平均测量来研究它们对热传导的影响,这些测量几乎没有提供关于单个晶界附近声子输运的信息。在这里,我们使用空间分辨时域热反射率(TDTR)测量与电子背散射衍射(EBSD)相结合,在硼掺杂多晶金刚石中单个晶界附近几微米范围内进行 κ 的局部测量。我们观察到晶界附近的热输运受到强烈抑制,κ 从大晶粒中心的约 1000 W m K 降低到晶界附近的约 400 W m K。此外,我们表明,这种 κ 的降低可以在距晶界约 10 μm 的范围内测量到。提出了一个理论模型,该模型捕获了由于无序晶界处强烈的声子扩散散射导致的声子平均自由程的局部减小。我们的结果为理解纳米材料中的声子-缺陷相互作用提供了一个新的框架,对于在电子热管理中使用高 κ 多晶材料作为热沉具有重要意义。