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Generation of hot electrons in nanostructures incorporating conventional and unconventional plasmonic materials

DOI:10.1039/c8fd00145f 期刊:Faraday Discussions 出版年份:2019 更新时间:2025-09-11 14:15:04
摘要: The generation of energetic electrons is an effect occurring in any plasmonic nanostructure. However, the number of electrons with high energies generated optically in a plasmonic nanostructure can be relatively small. This is an intrinsic property of the collective plasmon excitations in a Fermi gas of electrons. But the choices of material and geometry have a great impact on the generation rate, which are therefore crucial to design nanostructure with a large rate of generation of energetic (hot) electrons. Here we test different plasmonic materials from the point of view of the generation of hot electrons (HEs). Our choice of materials includes both strongly-plasmonic materials (Au, Ag, Cu and Al) and crystals with strongly broadened plasmonic resonances (Pt, TiN, ZrN). Regarding the choice of geometry, we consider two types of nanostructures, single nanocrystals deposited over a dielectric substrate and metastructure absorber, observing interesting opto-electronic properties. For single nanocrystals, the rate of HE generation is strongly material-dependent since the HE generation rate strongly depends on several physical parameters such as plasmonic enhancement, plasmonic resonance wavelength, Fermi energy, etc. Interestingly, the plasmonic meta-absorbers exhibit a different behaviour. The strongly-plasmonic metals, such as Au, Ag, Cu or Al, show very similar performances, while the materials with damped plasmon resonances demonstrate diverse and reduced rates of HE generation. The physical reason for these differentiated behaviours lies in the dielectric functions of these materials. In the metastructures, plasmonic resonances are in the infrared and the strongly-plasmonic materials behave as an almost ideal metal, whereas the second group of the materials exhibits strong dissipation. This makes the responses from the metastructures made of crystals with damped plasmons strongly dependent on the choice of material. The physical principles described in our study can be useful for designing metastructures and nanodevices based on HEs, which can be used in photo-chemistry and opto-electronics.
作者: Tianji Liu,Lucas V. Besteiro,Zhiming Wang,Alexander O. Govorov
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Investigating the generation of hot electrons in nanostructures incorporating conventional and unconventional plasmonic materials to design nanostructures with a large rate of generation of energetic (hot) electrons.

The study concludes that metastructures with a plasmonic mirror generate hot electrons more efficiently than single nanocrystals. Materials with broadened plasmonic peaks are less efficient for hot electron generation devices, yet some like TiN and ZrN are promising due to their cost-effectiveness. The physical principles described can be useful for designing efficient systems for hot electron generation in photo-chemistry and opto-electronics.

The study is computational and theoretical, relying on simulations rather than experimental validation. The practical implementation of the designed nanostructures and their performance in real-world applications may vary due to fabrication challenges and environmental factors.

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