Monitoring plasmonic hot-carrier chemical reactions at the single particle level

Simoncelli, Sabrina; Pensa, Evangelina; Brick, Thomas; Gargiulo, Julián; Lauri, Alberto; Cambiasso, Javier; Li, Yang; Maier, Stefan A.; Cortés, Emiliano

doi:10.1039/c8fd00138c

Cited by 31 publications

(32 citation statements)

References 47 publications

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“…Singleparticle photothermal approaches have been demonstrated for nanomaterials synthesis and could be useful, for example, for advancing nanothermolithography techniques, designing versatile optothermal nanophotonics devices, or conducting mechanistic studies in plasmonic catalysis. [56][57][58][59][60] Plasmonic NPs under mild illumination intensities represent a valuable platform for large-scale photothermal driven processes when considered in ensemble. Analogous to the distance dependence of the electric potential from a charged sphere, temperature drops relatively weakly as 1/r from the surface of a heated NP.…”

Section: Thermal Effects In Plasmonic Systemsmentioning

confidence: 99%

Challenges in Plasmonic Catalysis

et al. 2020

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The use of nanoplasmonics to control light and heat close to the thermodynamic limit enables exciting opportunities in the field of plasmonic catalysis. The decay of plasmonic excitations creates highly nonequilibrium distributions of hot carriers that can initiate or catalyze reactions through both thermal and nonthermal pathways. In this Perspective, we present the current understanding in the field of plasmonic catalysis, capturing vibrant debates in the literature, and discuss future avenues of exploration to overcome critical bottlenecks. Our Perspective spans first-principles theory and computation of correlated and far-from-equilibrium light-matter interactions, synthesis of new nanoplasmonic hybrids, and new steady-state and ultrafast spectroscopic probes of interactions in plasmonic catalysis, recognizing the key contributions of each discipline in realizing the promise of plasmonic catalysis. We conclude with our vision for fundamental and technological advances in the field of plasmon-driven chemical reactions in the coming years.

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Section: Thermal Effects In Plasmonic Systemsmentioning

confidence: 99%

Challenges in Plasmonic Catalysis

et al. 2020

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“…20 In the following, we review our efforts to understand, map and control chemical reactivity at the single plasmonic particle level. 29…”

Section: Figurementioning

confidence: 99%

From Optical to Chemical Hot Spots in Plasmonics

et al. 2019

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In recent years, the possibility to induce chemical transformations by using tunable plasmonic modes has opened the question of whether we can control or create chemical hot spots in these systems. This can be rationalized as the reactive analogue of the well-established concept of optical hot spots, which have drawn a great deal of attention to plasmonic nanostructures for their ability to circumvent the far-field diffraction limit of conventional optical elements. The parameters that determine the reactivity of plasmonic systems are deeply influenced by the dynamics and interplay of photons, plasmon-polaritons, carriers, phonons and molecular states. Although optical hot spots can be mainly defined by the geometry and permittivity of the nanostructures, the degrees of freedom influencing their photocatalytic properties appear to be much more numerous. These degrees of freedom can affect the reaction rates, the product selectivity or the spatial localization of a chemical reaction. In this Account, we show how the control of chemical hot spots can be achieved by carefully tuning the parameters that influence the cascade of events following the optical excitation of plasmonic modes in nanostructures. We discuss here a series of single photocatalyst techniques and ideas of how plasmonic nanoscale reactivity can be spatially mapped and imaged, and how the lifetime of hot and thermalized carriers can be altered by trap states on semiconductors and by metal-semiconductor interfaces. In addition, the tailored generation of non-thermal phonons in metallic nanostructures and their dissipation is shown as a promise to understand and exploit thermal photocatalysis at the nanoscale. Surpassing or enhancing each of these energy channels should enable to engineer solar nanometric photocatalysts. Nevertheless, the ultimate capability of a plasmonic photocatalyst to trigger a chemical reaction is correlated to its ability to navigate through, or even modify, the potential energy surface of a given chemical reaction. Here we reunite both worlds, the plasmonic photocatalysts and the molecular ones, identifying different energy transfer pathways and their influence on selectivity and efficiency of chemical reactions. We foresee that the migration from optical to chemical hot spots will greatly assist the understanding of ongoing plasmonic chemistry.

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“…Investigating such single nanostructures (or arrays of identical nanostructures) gives problems in detecting the small quantities of molecular product. While SERS techniques such as 19,28 maybe help in some cases, more developments in this area are also needed, in solution phase as well as gas phase catalysis. The challenge of fabricating nanostructures remains significant, since both atomic scale and nanoscale to wavelength-scale features are all important.…”

Section: Prospectsmentioning

confidence: 99%