The fluorescence response of a chromophore in the proximity of a plasmonic nanostructure can be enhanced by several orders of magnitude, yielding the so-called surface-enhanced fluorescence (SEF). An in-depth understanding of SEF mechanisms benefits from fully atomistic theoretical models because SEF signals can be non-trivially affected by the atomistic profile of the nanostructure's surface. This work presents the first fully atomistic multiscale approach to SEF, capable of describing realistic structures. The method is based on coupling density functional theory (DFT) with state-of-the-art atomistic electromagnetic approaches, allowing for reliable physically-based modeling of molecule–nanostructure interactions. Computed results remarkably demonstrate the key role of the NP morphology and atomistic features in quenching/enhancing the fluorescence signal.

Multiscale Modeling of Surface Enhanced Fluorescence

Chiara Cappelli
;
Pablo Grobas Illobre;Piero Lafiosca;Teresa Guidone;Francesco Mazza;Tommaso Giovannini
2024

Abstract

The fluorescence response of a chromophore in the proximity of a plasmonic nanostructure can be enhanced by several orders of magnitude, yielding the so-called surface-enhanced fluorescence (SEF). An in-depth understanding of SEF mechanisms benefits from fully atomistic theoretical models because SEF signals can be non-trivially affected by the atomistic profile of the nanostructure's surface. This work presents the first fully atomistic multiscale approach to SEF, capable of describing realistic structures. The method is based on coupling density functional theory (DFT) with state-of-the-art atomistic electromagnetic approaches, allowing for reliable physically-based modeling of molecule–nanostructure interactions. Computed results remarkably demonstrate the key role of the NP morphology and atomistic features in quenching/enhancing the fluorescence signal.
2024
Settore CHIM/02 - Chimica Fisica
   PNRR Partenariati Estesi - NQSTI - National Quantum Science and Technology Institute.
   Ministero della pubblica istruzione, dell'università e della ricerca
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11384/142204
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