Theoretical predictions for hot-carrier generation from surface plasmon decay

By Ravishankar Sundararaman, Prineha Narang, Adam S. Jermyn, W. Goddard III, Harry A. Atwater. Nature Communications, 2014

693 citations recorded by the source corpus.

Decay of surface plasmons to hot carriers finds a wide variety of applications in energy conversion, photocatalysis and photodetection. However, a detailed theoretical description of plasmonic hot-carrier generation in real materials has remained incomplete. Here we report predictions for the prompt distributions of excited ‘hot’ electrons and holes generated by plasmon decay, before inelastic relaxation, using a quantized plasmon model with detailed electronic structure. We find that carrier energy distributions are sensitive to the electronic band structure of the metal: gold and copper produce holes hotter than electrons by 1–2 eV, while silver and aluminium distribute energies more equitably between electrons and holes. Momentum-direction distributions for hot carriers are anisotropic, dominated by the plasmon polarization for aluminium and by the crystal orientation for noble metals. We show that in thin metallic films intraband transitions can alter the carrier distributions, producing hotter electrons in gold, but interband transitions remain dominant. A full theoretical understanding of plasmon decay into hot carriers will help in applications such as solar cells or photocatalysis. Here, the authors present a quantized plasmon model to calculate the hot-carrier distribution from plasmon decay and show its sensitivity to the band structure of the host metal.

Subfields: Biomedical Engineering, Electronic, Optical and Magnetic Materials, Materials Chemistry

View Paper: https://www.semanticscholar.org/paper/36eaa1862e18a0b15885e7363e8d5195ebdf07e9

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Citations in the corpus

Quantum Plasmonics (2016, methodology): “Recently, the decay of surface plasmons via direct transitions in the bulk material has been examined in detail using Fermi’s golden rule calculations on relativistic DFTþ U band structures [108] and confirmed by subsequent GW calculations [155].”