Nonlinear Plasmonics in Nanostructured Phosphorene

Phosphorene has emerged as an atomically thin platform for optoelectronics and nanophotonics due to its excellent optical properties and the possibility of actively tuning light-matter interactions through electrical doping. While phosphorene is a two-dimensional semiconductor, plasmon resonances characterized by pronounced anisotropy and strong optical confinement are anticipated to emerge in highly doped samples. Here we show that the localized plasmons supported by phosphorene nanoribbons (PNRs) exhibit high tunability in relation to both edge termination and doping charge polarity and can trigger an intense nonlinear optical response at moderate doping levels. Our explorations are based on a second-principles theoretical framework, employing maximally localized Wannier functions constructed from ab initio electronic structure calculations, which we introduce here to describe the linear and nonlinear optical response of PNRs on mesoscopic length scales. Atomistic simulations reveal the high tunability of plasmons in doped PNRs at near-infrared frequencies, which can facilitate the synergy between the electronic band structure and plasmonic field confinement to drive efficient high-harmonic generation. Our findings establish nanostructured phosphorene as a versatile atomically thin material candidate for nonlinear plasmonics.

Automated summary

Phosphorene, an atomically thin material, has garnered significant attention in the fields of optoelectronics and nanophotonics due to its exceptional optical properties and the ability to actively control light-matter interactions through electrical doping. Researchers have discovered that localized plasmons supported by phosphorene nanoribbons exhibit high tunability in relation to edge termination and doping charge polarity, leading to intense nonlinear optical responses at moderate doping levels. The tunability of plasmons in doped phosphorene nanoribbons at near-infrared frequencies can facilitate efficient high-harmonic generation by combining the electronic band structure and plasmonic field confinement.