Ab initio quantum dynamics of plasmonic charge carriers
Ab initio quantum dynamics of plasmonic charge carriers
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DOI：
10.1016/j.trechm.2023.02.010
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发表时间：
2023-03
影响因子：
15.7
通讯作者：
Wei Li;Ting Xue;Carlos Mora-Perez;O. Prezhdo
中科院分区：
文献类型：
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作者：
Wei Li;Ting Xue;Carlos Mora-Perez;O. Prezhdo
表面等离子体对电场有强烈的响应，并产生可用于光电子器件的高能(热载流子)载流子。然而，热载流子的利用必须超过金属中的快速载流子弛豫。通常，基于等离子体激元激发的纳米级器件的报道效率很低，并且器件运行的机制在该领域内仍然不一致。进一步的发展取决于对等离子激元衰变过程的本质和动力学的基本理解。我们提供了热载流子动力学的时间域初始模型的概述，证明了等离子体材料表面结构的原子细节，以及它们与半导体和分子电荷接受者和衬底的化学相互作用，在控制动力学途径中起着关键作用。所考虑的案例研究代表了各种动力学渠道，并说明了太阳能和光电子的应用。
Surface plasmons respond strongly to electric fields and generate energetic (hot) charge carriers that can be used in optoelectronic devices. However, utilization of hot carriers has to outcompete fast carrier relaxation in metals. Often, the reported efficiencies of nanoscale devices based on plasmon excitations are low and the mechanisms of device operation remain inconsistent within the field. Further developments hinge on fundamental understanding of the nature and kinetics of plasmon decay processes. We provide an overview of time domainab initiomodeling of hot carrier dynamics, demonstrating that atomistic details of the surface structure of plasmonic materials, and their chemical interaction with semiconducting and molecular charge acceptors and substrates, play key roles in governing the dynamics pathways. Considered case studies represent various dynamics channels and illustrate solar energy and optoelectronic applications.