Electron–Phonon Coupling in Current-Driven Single-Molecule Junctions,Journal of the American Chemical Society

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Electron–Phonon Coupling in Current-Driven Single-Molecule Junctions
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-02-04 , DOI: 10.1021/jacs.9b07757
Hai Bi ₁ , Carlos-Andres Palma _{1,

2,

3} , Yuxiang Gong ₁ , Klara Stallhofer ₁ , Matthias Nuber ₁ , Chao Jing ₁ , Felix Meggendorfer ₁ , Shizheng Wen ₄ , ChiYung Yam ₄ , Reinhard Kienberger ₁ , Mark Elbing ₅ , Marcel Mayor _{6,

7} , Hristo Iglev ₁ , Johannes V Barth ₁ , Joachim Reichert ₁

Affiliation

Vibrational excitations provoked by coupling effects during charge transport through single molecules are intrinsic energy dissipation phenomena, in close analogy to electron-phonon coupling in solids. One fundamental challenge in molecular electronics is the quantitative determination of charge-vibrational (electron-phonon) coupling for single-molecule junctions. The ability to record electron-phonon coupling phenomena at the single-molecule level is a key prerequisite to fully rationalize and optimize charge-transport efficiencies for specific molecular configurations and currents. Here we exemplarily determine the pertaining coupling characteristics for a current-carrying chemically well-defined molecule by synchronous vibrational and current-voltage spectroscopy. These metal-molecule-metal junction insights are complemented by time-resolved infrared spectroscopy to assess the intramolecular vibrational relaxation dynamics. By measuring and analyzing the steady-state vibrational distribution during transient charge transport in a bis-phenylethynyl-anthracene derivative using anti-Stokes Raman scattering, we find ∼0.5 vibrational excitations per elementary charge passing through the metal-molecule-metal junction, by means of a rate model ansatz and quantum-chemical calculations.

中文翻译：

电流驱动单分子结中的电子-声子耦合

在通过单个分子的电荷传输过程中由耦合效应引起的振动激发是固有的能量耗散现象，与固体中的电子-声子耦合非常相似。分子电子学的一项基本挑战是定量测定单分子结的电荷-振动（电子-声子）耦合。在单分子水平记录电子-声子耦合现象的能力是完全合理化和优化特定分子配置和电流的电荷传输效率的关键先决条件。在这里，我们通过同步振动和电流 - 电压光谱示例性地确定了载流化学明确定义的分子的相关耦合特性。这些金属-分子-金属结的洞察力与时间分辨红外光谱相辅相成，以评估分子内振动弛豫动力学。通过使用反斯托克斯拉曼散射测量和分析双苯乙炔基蒽衍生物中瞬态电荷传输过程中的稳态振动分布，我们发现通过金属-分子-金属结的每个基本电荷约有 0.5 个振动激发率模型 ansatz 和量子化学计算。

更新日期：2020-02-04

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