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arXiv 2005.10932cond-mat.mtrl-sci
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量子化等离子体激元在银纳米粒子中产生热载流子的介电工程

Dielectric engineering of hot carrier generation by quantized plasmons in embedded silver nanoparticles

Lara Román Castellanos, Ortwin Hess, Johannes Lischner

摘要:

了解和控制等离子体激元诱导的热载流子的性质是迈向下一代光伏和光催化器件的关键一步。在这里,我们发现了一条路线,工程热载流子生成率的银纳米粒子设计嵌入在介电基质材料。扩展我们最近建立的量子力学方法来描述量子化等离子体的衰变成热载流子,我们捕获的纳米粒子环境和银d-电子通过有效的电子-电子相互作用的内部屏蔽的外部屏蔽。我们发现,热载流子的产生可以最大限度地通过工程的介电主体材料,使局部表面等离子体激元的能量与最高值的纳米粒子联合态密度相一致。这使我们能够揭示一条控制载流子能量和产生量的途径,例如通过嵌入强屏蔽环境中获得大量相对低能量的载流子。

英文摘要:

Understanding and controlling properties of plasmon-induced hot carriers is a key step towards next-generation photovoltaic and photocatalytic devices. Here, we uncover a route to engineering hot-carrier generation rates of silver nanoparticles by designed embedding in dielectric host materials. Extending our recently established quantum-mechanical approach to describe the decay of quantized plasmons into hot carriers we capture both external screening by the nanoparticle environment and internal screening by silver d-electrons through an effective electron-electron interaction. We find that hot-carrier generation can be maximized by engineering the dielectric host material such that the energy of the localized surface plasmon coincides with the highest value of the nanoparticle joint density of states. This allows us to uncover a path to control the energy of the carriers and the amount produced, for example a large number of relatively low-energy carriers are obtained by embedding in strongly screening environments.

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