Abstract
AbstractAccurate complex dielectric functions are critical to accelerate the development of rationally designed metal alloy systems for nanophotonic applications, and to thereby unlock the potential of alloying for tailoring nanostructure optical properties. To date, however, accurate alloy dielectric functions are widely lacking. Here, a time‐dependent density‐functional theory computational framework is employed to compute a comprehensive binary alloy dielectric function library for the late transition metals most commonly employed in plasmonics (Ag, Au, Cu, Pd, Pt). Excellent agreement is found between electrodynamic simulations based on these dielectric functions and selected alloy systems experimentally scrutinized in 10 at% composition intervals. Furthermore, it is demonstrated that the dielectric functions can vary in very non‐linear fashion with composition, which paves the way for non‐trivial optical response optimization by tailoring material composition. The presented dielectric function library is thus a key resource for the development of alloy nanomaterials for applications in nanophotonics, optical sensors, and photocatalysis.
Highlights
Comparing the experimentally determined plasmonic resonance peak descriptors spectral position and full width at half maximum (FWHM) with finite-difference timedomain (FDTD) electrodynamic simulations using the dielectric functions (DFs) obtained by first-principles calculations as input (Figure 1c–e), we find excellent agreement and validate our approach
It is very important to emphasize the large variations in the experimental data and the large number of different measurements and techniques that are required to span the entire spectral range considered in our calculations
We have from first principles calculated DFs for the ten binary alloys formed by combinations of the most common metals used in plasmonics, Ag, Au, Cu, Pd, and Pt, and found excellent agreement between the experimentally measured optical response of nanofabricated nanodisk arrays of four selected alloy systems (Ag–Au, Au–Cu, Au–Pd, Ag–Pd), and corresponding electrodynamic simulations using the computed DFs as key input
Summary
It was not until very recently, enabled by the development of the corresponding nanofabrication methods, that systematic investigations of the fundamental properties of noble metal alloy nanostrucdynamic simulations based on these dielectric functions and selected alloy sys- tures started to appear.[2,3,4,5,6,7,8,9,10] Some of these tems experimentally scrutinized in 10 at% composition intervals. The presented dielectric funcmaterials have already found applications, for example in plasmonic hydrogen sensors,[11,12] or are suggested for the use in plasmon-mediated catalysis.[13] Despite these successful initial efforts tion library is a key resource for the development of alloy nanomaterials in establishing alloying as a new handle for applications in nanophotonics, optical sensors, and photocatalysis. Introduction of alloys at the atomic level, as well as the limited availability of reliable complex dielectric functions (DFs) of metal alloys
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