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德鲁德金属的“热”光致发光理论。

Theory of "Hot" Photoluminescence from Drude Metals.

作者信息

Sivan Yonatan, Dubi Yonatan

机构信息

School of Electrical and Computer Engineering, Ben-Gurion University of the Negev, Be'er sheva, Israel 8410501.

Department of Chemistry, Ben-Gurion University of the Negev, Be'er sheva, Israel 8410501.

出版信息

ACS Nano. 2021 May 25;15(5):8724-8732. doi: 10.1021/acsnano.1c00835. Epub 2021 Apr 27.

Abstract

We provide a complete quantitative theory for light emission from Drude metals under continuous wave illumination, based on our recently derived steady-state nonequilibrium electron distribution. We show that the electronic contribution to the emission exhibits a dependence on the emission frequency which is very similar to the energy dependence of the nonequilibrium distribution, and characterize different scenarios determining the measurable emission line shape. This enables the identification of experimentally relevant situations, where the emission lineshapes deviate significantly from predictions based on the standard theory (namely, on the photonic density of states), and enables the differentiation between cases where the emission scales with the metal object surface or with its volume. We also provide an analytic description (which is absent from the literature) of the (polynomial) dependence of the metal emission on the electric field, its dependence on the pump laser frequency, and its nontrivial exponential dependence on the electron temperature, both for the Stokes and anti-Stokes regimes. Our results imply that the emission does not originate from either Fermion statistics (due to - interactions), and even though one could have expected the emission to follow boson statistics due to involvement of photons (as in Planck's Black Body emission), it turns out that it deviates from that form as well. Finally, we resolve the arguments associated with the effects of electron and lattice temperatures on the emission, and which of them can be extracted from the anti-Stokes emission.

摘要

基于我们最近推导出的稳态非平衡电子分布,我们为连续波照射下德鲁德金属的光发射提供了一个完整的定量理论。我们表明,电子对发射的贡献表现出对发射频率的依赖性,这与非平衡分布的能量依赖性非常相似,并表征了决定可测量发射线形状的不同情况。这使得能够识别实验相关的情况,即发射线形状与基于标准理论(即基于光子态密度)的预测有显著偏差的情况,并能够区分发射与金属物体表面或其体积成比例的情况。我们还提供了一种解析描述(文献中未出现),用于描述金属发射对电场的(多项式)依赖性、对泵浦激光频率的依赖性以及对电子温度的非平凡指数依赖性,涵盖斯托克斯和反斯托克斯两种情况。我们的结果表明,发射并非源于费米子统计(由于 - 相互作用),而且尽管由于光子的参与(如普朗克黑体发射那样)人们可能预期发射遵循玻色子统计,但事实证明它也偏离了那种形式。最后,我们解决了与电子和晶格温度对发射的影响相关的争论,以及其中哪些可以从反斯托克斯发射中提取出来。

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