Nonlinear optical processes resulting from the interaction of light with matter have provided great opportunities in photonics technologies by enabling spectral control of light. Here, based on first-principles calculations, we investigate the linear and nonlinear optical response of monolayer hBN in the mid-infrared polaritonic region following time-domain and perturbative schemes, from which we conclude an extraordinarily large nonlinear response, which can be modulated by lateral electrical gating and presents an opportunity to achieve quantum blockade at the level of a few quanta. Our study reveals a range of potential applications that include harmonic generation, optical modulation, and quantum information in the mid-infrared range.
Nonlinear optical processes resulting from light-matter interaction are essential for control of light by light in photonic technologies. Here, based on first-principles calculations, we investigate the linear and nonlinear optical response of monolayer hBN in the mid-infrared polaritonic region following time-domain and perturbative schemes, from which we conclude an extraordinarily large nonlinear response, which can be modulated by lateral electrical gating and presents an opportunity to achieve quantum blockade at the level of a few quanta. Our study reveals a range of potential applications that include harmonic generation, optical modulation, and quantum information in the mid-infrared range.
Recent progress in the fabrication of metallic thin films allows for a precise control of the surface crystallographic orientation and thickness, turning them to be a great appeal in plasmonic devices. Considering such a crystalline quality and going towards smaller optical designs; surface, nonlocal, and quantum finite-size effects play a major role in metallic thin films when interacting with light. Here we explore various strategies to seek for the linear and nonlinear optical response manifested in a variety of scenarios and configurations which are based on precise quantum-mechanical formalisms that describe the dynamics of electrons in such films, e.g. EELS, Feibelman d-parameters, periodic- and finite-systems, etc. We believe that our results can inspire future devices based on crystalline metal films as well as motivate further numerical implementation strategies.
Recent progress in the fabrication of metallic thin films allows for precise control of the surface crystallographic orientation and thickness, turning them to be a great appeal in plasmonic devices. Considering such a crystalline quality and going towards smaller optical designs; surface, nonlocal, and quantum finite-size effects play a major role in metallic thin films when interacting with light. Here we explore various strategies to seek for the linear and nonlinear optical response manifested in a variety of scenarios and configurations which are based on precise quantum-mechanical formalisms that describe the dynamics of electrons in such films, e.g. EELS, Feibelman d-parameters, periodic- and finite-systems, etc. We believe that our results can inspire future devices based on crystalline metal films as well as motivate further numerical implementation strategies.
Atomically thin films possess appealing intrinsic properties for nonlinear optics that we explore employing a rigorous quantum-mechanical description. The main optical response is driven by plasmons, the collective oscillation of conduction electrons, which are modeled through the proper consideration of the dominant features of their electronic band structure, including surface and quantum well states along with the bandgap arising for each crystallographic facet. We report a beneficial use of films decreasing in thickness down to few-atom-thick sizes, influencing both the linear and the nonlinear optical response. Such a degree of tunability makes them unique together with lower losses compared to their amorphous counterparts. These results facilitate the development of atomically-thin nonlinear nanophotonic devices based on well-defined crystalline metal films.
The nonlocal response associated with the collective oscillation of conduction electrons (plasmons) in atomically thin films plays a significant role in the optical response. Here we exploit the use of surface plasmons to characterize the nonlinear optical behavior of few atom-thick films. The results show beneficial use of thinner films that are computed employing a full quantum mechanical model that incorporates details of the crystallographic orientation allowing us to exploit the facets (111) and (100) in the random phase approximation. These results facilitate the fabrication of nanophotonic devices based on crystalline metals films which offer lower losses than their amorphous counterparts.
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