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doi: 10.1002/adma.202209100 , 10.14279/depositonce-17645 , 10.17169/refubium-37723 , 10.17863/cam.92389 , 10.48550/arxiv.2211.04615
pmid: 36482148
arXiv: 2211.04615
AbstractHybrid plasmonic devices involve a nanostructured metal supporting localized surface plasmons to amplify light–matter interaction, and a non‐plasmonic material to functionalize charge excitations. Application‐relevant epitaxial heterostructures, however, give rise to ballistic ultrafast dynamics that challenge the conventional semiclassical understanding of unidirectional nanometal‐to‐substrate energy transfer. Epitaxial Au nanoislands are studied on WSe2 with time‐ and angle‐resolved photoemission spectroscopy and femtosecond electron diffraction: this combination of techniques resolves material, energy, and momentum of charge‐carriers and phonons excited in the heterostructure. A strong non‐linear plasmon–exciton interaction that transfers the energy of sub‐bandgap photons very efficiently to the semiconductor is observed, leaving the metal cold until non‐radiative exciton recombination heats the nanoparticles on hundreds of femtoseconds timescales. The results resolve a multi‐directional energy exchange on timescales shorter than the electronic thermalization of the nanometal. Electron–phonon coupling and diffusive charge‐transfer determine the subsequent energy flow. This complex dynamics opens perspectives for optoelectronic and photocatalytic applications, while providing a constraining experimental testbed for state‐of‐the‐art modelling.
[PHYS]Physics [physics], excitons, Condensed Matter - Mesoscale and Nanoscale Physics, interfacial charge transfer, transition metal dichalcogenides, 500 Naturwissenschaften und Mathematik::530 Physik::530 Physik, FOS: Physical sciences, 530, ultrafast energy transfer, 600 Technik, Medizin, angewandte Wissenschaften::660 Chemische Verfahrenstechnik::660 Chemische Verfahrenstechnik, light–matter interactions, [PHYS] Physics [physics], Mesoscale and Nanoscale Physics (cond-mat.mes-hall), light-matter interactions, hybrid plasmonics, plasmons, femtosecond electron diffraction, 2D semiconductors
[PHYS]Physics [physics], excitons, Condensed Matter - Mesoscale and Nanoscale Physics, interfacial charge transfer, transition metal dichalcogenides, 500 Naturwissenschaften und Mathematik::530 Physik::530 Physik, FOS: Physical sciences, 530, ultrafast energy transfer, 600 Technik, Medizin, angewandte Wissenschaften::660 Chemische Verfahrenstechnik::660 Chemische Verfahrenstechnik, light–matter interactions, [PHYS] Physics [physics], Mesoscale and Nanoscale Physics (cond-mat.mes-hall), light-matter interactions, hybrid plasmonics, plasmons, femtosecond electron diffraction, 2D semiconductors
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