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Band alignment and defects influence the electron-phonon heat transport mechanisms across metal interfaces

机译:带对准和缺陷会影响跨金属界面的电子 - 声子热传输机制

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摘要

We report on the experimental determination of electron-electron conductance at Au/TiO_x interfacial regions and electron-phonon coupling of thin TiO_x layers for x = 0-2.62. Our study demonstrates that the electronic energy transport mechanisms at metal/metal oxide interfaces are enhanced through metallic defects that lead to electronic band alignment between the metal and metal oxide (in our case, Au and TiO_x). Electronic heat transport processes are interrogated via a pump/probe technique, utilizing sub-picosecond laser pulses to monitor the ultrafast thermoreflectance responses of Au/TiO_x systems, which were analyzed using a two-temperature model to extract electron-electron conductances at Au/TiO_x interfaces and the electron-phonon coupling in TiO_x layers. We find that TiO_x stoichiometries near TiO_2 have ultrahigh electron-phonon coupling factors similar to that of pure Ti and that electronic energy transmission from Au to TiO_x layers is comparable to that of Au to Ti due to the presence of Ti~0 defects. For x = 2.62 in TiO_x, electron-phonon coupling is reduced by more than a factor of 5. Our experimental data are corroborated by real-time time-dependent density functional theory calculations, which show that excited electrons in Au do not participate in the TiO_x phonon relaxation process, resulting in lower electron-electron energy transmission from Au and electron-phonon coupling due to the difference in the Fermi energy of Au relative to the conduction band minimum of TiO_x when x >2.
机译:我们报告了X = 0-2.62的薄TiO_x层的Au / TiO_x界面区域和电子 - 声子耦合的实验测定。我们的研究表明,通过金属缺陷导致金属和金属氧化物(在我们的情况下,Au和TiO_x)之间的金属缺陷来增强金属/金属氧化物界面处的电子能量传输机制。通过泵/探针技术询问电子热传输过程,利用子皮秒激光脉冲来监测Au / TiO_x系统的超快热反应响应,其使用两个温度模型分析以提取Au / TiO_x的电子导电接口和TiO_x层中的耦合器耦合。我们发现TiO_2附近的TiO_X的化学测定仪具有类似于纯TI的超高电子 - 声子耦合因子,并且由于Ti〜0缺陷的存在,来自Au至TiO_x层的电子能量传输与Au至Ti的电子能量传输相当。对于TiO_x中的x = 2.62,电子 - 声子耦合减小超过5倍5.我们的实验数据通过实时时间依赖的密度泛函理论计算来证实,这表明AU中的激发电子不参加TiO_X声子放宽过程,导致来自Au和电子 - 声子耦合的较低电子能量传递,由于Au的Fermi能量相对于X> 2时的导通带的传导频带的差异。

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  • 来源
    《Applied Physics Letters》 |2021年第16期|163503.1-163503.7|共7页
  • 作者单位

    Department of Mechanical and Aerospace Engineering University of Virginia Charlottesville Virginia 22904 USA;

    Department of Materials Science and Engineering University of Virginia Charlottesville Virginia 22904 USA;

    Department of Mechanical and Aerospace Engineering University of Virginia Charlottesville Virginia 22904 USA;

    School of Materials Science and Engineering Dalian Jiaotong University Dalian 116028 Liaoning Province China;

    Department of Chemistry University of Southern California Los Angeles California 90089 USA;

    Department of Materials Science and Engineering University of Virginia Charlottesville Virginia 22904 USA;

    Department of Mechanical and Aerospace Engineering University of Virginia Charlottesville Virginia 22904 USA Department of Materials Science and Engineering University of Virginia Charlottesville Virginia 22904 USA Department of Physics University of Virginia Charlottesville Virginia 22904 USA;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);
  • 原文格式 PDF
  • 正文语种 eng
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