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Quantum-mechanical effects in photoluminescence from thin crystalline gold films

Light(Science & Applications) 2024年第4期13卷 783-794页

作者： Alan R.Bowman Alvaro Rodríguez Echarri Fatemeh Kiani fadil iyikanat Ted V.Tsoulos Joel D.Cox Ravishankar Sundararaman F.Javier García de Abajo Giulia Tagliabue Laboratory of Nanoscience for Energy Technologies(LNET) STIÉcole Polytechnique Fédérale de Lausanne(EPFL)LausanneSwitzerland ICFO–Institut de Ciencies Fotoniques The Barcelona Institute of Science and TechnologyCastelldefels(Barcelona)Spain. MBI–Max-Born-Institut BerlinGermany. POLIMA–Center for Polariton-driven Light–Matter Interactions University of Southern DenmarkOdense MDenmark. Danish Institute for Advanced Study University of Southern DenmarkOdense MDenmark. Department of Materials Science&Engineering Rensselaer Polytechnic InstituteTroyNYUSA. Department of Physics Applied Physicsand AstronomyRensselaer Polytechnic InstituteTroyNYUSA. ICREA–Institucio Catalana de Recerca i Estudis Avancats BarcelonaSpain

Luminescence constitutes a unique source of insight into hot carrier processes in metals,including those in plasmonic nanostructures used for sensing and energy ***,being weak in nature,metal luminescence remains poorly understood,its microscopic origin strongly debated,and its potential for unraveling nanoscale carrier dynamics largely ***,we reveal quantum-mechanical effects in the luminescence emanating from thin monocrystalline gold ***,we present experimental evidence,supported by first-principles simulations,to demonstrate its photoluminescence origin(i.e.,radiative emission from electron/hole recombination)when exciting in the interband *** model allows us to identify changes to the measured gold luminescence due to quantum-mechanical effects as the gold film thickness is ***,such effects are observable in the luminescence signal from flakes up to 40 nm in thickness,associated with the out-of-plane discreteness of the electronic band structure near the Fermi *** qualitatively reproduce the observations with first-principles modeling,thus establishing a unified description of luminescence in gold monocrystalline flakes and enabling its widespread application as a probe of carrier dynamics and light-matter interactions in this *** study paves the way for future explorations of hot carriers and charge-transfer dynamics in a multitude of material systems.

关键词： luminescence quantum crystalline

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