Hot Carrier Distribution Engineering by Alloying: Picking Elements for the Desired Purposes

Metal alloys hold the promise of providing hot carrier generation distributions superior to pure metals in applications such as sensing, catalysis, and solar energy harvesting. Guidelines for finding the optimal alloy configuration for a target application require an understanding of the connection between alloy composition and hot carrier distribution. Here, we present a density functional theory (DFT)-based computational approach to investigate the photogenerated hot carrier distribution of metal alloys based on the joint density of states and the electronic structure. We classified the metals by their electronic structure into closed d-shell, open d-shell, p-block, and s-block elements. It is shown that combining closed d-shell elements enables modulation of the distribution of highly energetic holes typical of pure metals but also leads to hot carrier production by infrared (IR) light excitation and the appearance of highly energetic electrons due to band folding and splitting. This feature arises as an emergent property of alloying and is unveiled only when the hot carrier distribution computation takes momentum conservation into account. The combination of closed d-shell with open d-shell elements allows an abundant production of hot carriers in a broad energy range, while alloying a closed d-shell element with an s-block element opens the door to hot electron distribution skewed toward high-energy electrons. The combination of the d-shell with the p-block elements results in a moderate hot carrier distribution whose asymmetry can be tuned by composition. Overall, the obtained insights that connect alloy composition, band structure, and resulting carrier distribution provide a toolkit to match elements in an alloy for the deliberate engineering of hot carrier distribution

Dark Modes and Fano Resonances in Plasmonic Clusters Excited by Cylindrical Vector Beams

Control of the polarization distribution of light allows tailoring the electromagnetic response of plasmonic particles. By rigorously extending the generalized multiparticle Mie theory, we show that focused cylindrical vector beams (CVB) can be used to efficiently excite dark plasmon modes in nanoparticle clusters. In addition to the small radiative damping and large field enhancement associated to dark modes, excitation with CVB can give place to unusual phenomenology like the formation of electromagnetic cold spots and the generation of Fano resonances in highly symmetric clusters. Overall, the results show the potential of CVB to tailor the plasmonic response of nanoparticle clusters in a unique way

Dark Modes and Fano Resonances in Plasmonic Clusters Excited by Cylindrical Vector Beams

Control of the polarization distribution of light allows tailoring the electromagnetic response of plasmonic particles. By rigorously extending the generalized multiparticle Mie theory, we show that focused cylindrical vector beams (CVB) can be used to efficiently excite dark plasmon modes in nanoparticle clusters. In addition to the small radiative damping and large field enhancement associated to dark modes, excitation with CVB can give place to unusual phenomenology like the formation of electromagnetic cold spots and the generation of Fano resonances in highly symmetric clusters. Overall, the results show the potential of CVB to tailor the plasmonic response of nanoparticle clusters in a unique way

Dark Modes and Fano Resonances in Plasmonic Clusters Excited by Cylindrical Vector Beams

Control of the polarization distribution of light allows tailoring the electromagnetic response of plasmonic particles. By rigorously extending the generalized multiparticle Mie theory, we show that focused cylindrical vector beams (CVB) can be used to efficiently excite dark plasmon modes in nanoparticle clusters. In addition to the small radiative damping and large field enhancement associated to dark modes, excitation with CVB can give place to unusual phenomenology like the formation of electromagnetic cold spots and the generation of Fano resonances in highly symmetric clusters. Overall, the results show the potential of CVB to tailor the plasmonic response of nanoparticle clusters in a unique way

Dark Modes and Fano Resonances in Plasmonic Clusters Excited by Cylindrical Vector Beams

Control of the polarization distribution of light allows tailoring the electromagnetic response of plasmonic particles. By rigorously extending the generalized multiparticle Mie theory, we show that focused cylindrical vector beams (CVB) can be used to efficiently excite dark plasmon modes in nanoparticle clusters. In addition to the small radiative damping and large field enhancement associated to dark modes, excitation with CVB can give place to unusual phenomenology like the formation of electromagnetic cold spots and the generation of Fano resonances in highly symmetric clusters. Overall, the results show the potential of CVB to tailor the plasmonic response of nanoparticle clusters in a unique way

Die Operationstechnik der erweiterten endonasalen Kieferhöhlenoperation

We report the fine-tuning of the localized surface plasmon resonances (LSPRs) from ultraviolet to near-infrared by nanoengineering the metal nanoparticle morphologies from solid Ag nanocubes to hollow AuAg nanoboxes and AuAg nanoframes. Spatially resolved mapping of plasmon resonances by electron energy loss spectroscopy (EELS) revealed a homogeneous distribution of highly intense plasmon resonances around the hollow nanostructures and the interaction, that is, hybridization, of inner and outer plasmon fields for the nanoframe. Experimental findings are accurately correlated with the boundary element method (BEM) simulations demonstrating that the homogeneous distribution of the plasmon resonances is the key factor for their improved plasmonic properties. As a proof of concept for these enhanced plasmonic properties, we show the effective label free sensing of bovine serum albumin (BSA) of single-walled AuAg nanoboxes in comparison with solid Au nanoparticles, demonstrating their excellent performance for future biomedical applications