Strong-Field Control of Plasmonic Properties in Core–Shell Nanoparticles

Utilization of the plasmonic response in nanosystems is a key component of nanophotonics that is typically altered by varying the incident optical frequency or the material configuration. However, in this work we demonstrate that employing intense, femtosecond laser fields unlock nonlinear light–mat...

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Bibliographic Details
Published in:ACS photonics 2022-11, Vol.9 (11), p.3515-3521
Main Authors: Powell, Jeffrey A., Li, Jianxiong, Summers, Adam, Robatjazi, Seyyed Javad, Davino, Michael, Rupp, Philipp, Saydanzad, Erfan, Sorensen, Christopher M., Rolles, Daniel, Kling, Matthias F., Trallero, Carlos, Thumm, Uwe, Rudenko, Artem
Format: Article
Language:English
Subjects:
energy
femtosecond laser
gold
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
nanoparticles
nanoplasmonics
nanospheres
nonlinear optics
photoelectron spectroscopy
plasmonics
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Summary:Utilization of the plasmonic response in nanosystems is a key component of nanophotonics that is typically altered by varying the incident optical frequency or the material configuration. However, in this work we demonstrate that employing intense, femtosecond laser fields unlock nonlinear light–matter interactions such that precise control of the optical response is achieved solely by adjusting the incident intensity. The plasmonic properties of Au/SiO2 nanoshells are manipulated by exploiting the nonlinear index of refraction of gold and experimentally observed by employing photoelectrons emitted during the interaction as a sensitive, sub-wavelength probe. A striking transition seen in the photoelectron energy spectrum between the weak and strong-field regime is verified by a modified Mie theory simulation that incorporates the nonlinear dielectric nanoshell response. The exhibited intensity-dependent optical control of the plasmonic response in prototypical core–shell nanoparticles paves the way toward ultrafast switching and opto-electronic signal modulation with more complex nanostructures.
ISSN:2330-4022
2330-4022
DOI:10.1021/acsphotonics.2c00663