Nonlinear Interactions between Free Electrons and Nanographenes

Free electrons act as a source of highly confined, spectrally broad optical fields that are widely used to map photonic modes with nanometer/millielectronvolt space/energy resolution through currently available electron energy-loss and cathodoluminescence spectroscopies. These techniques are underst...

ver descrição completa

Detalhes bibliográficos
Autores: Cox, Joel D., García de Abajo, Francisco Javier
Formato: artículo
Fecha de publicación:2020
País:España
Recursos:Universitat Politècnica de Catalunya (UPC)
Repositorio:UPCommons. Portal del coneixement obert de la UPC
Idioma:inglés
OAI Identifier:oai:upcommons.upc.edu:2117/348822
Acesso em linha:https://hdl.handle.net/2117/348822
https://dx.doi.org/10.1021/acs.nanolett.0c00538
Access Level:acceso abierto
Palavra-chave:Graphene
Grafè
Àrees temàtiques de la UPC::Física
Descrição
Resumo:Free electrons act as a source of highly confined, spectrally broad optical fields that are widely used to map photonic modes with nanometer/millielectronvolt space/energy resolution through currently available electron energy-loss and cathodoluminescence spectroscopies. These techniques are understood as probes of the linear optical response, while nonlinear dynamics has escaped observation with similar degree of spatial detail, despite the strong enhancement of the electron evanescent field with decreasing electron energy. Here, we show that the field accompanying low-energy electrons can trigger anharmonic response in strongly nonlinear materials. Specifically, through realistic quantum-mechanical simulations, we find that the interaction between ≲100 eV electrons and plasmons in graphene nanostructures gives rise to substantial optical nonlinearities that are discernible as saturation and spectral shifts in the plasmonic features revealed in the cathodoluminescence emission and electron energy-loss spectra. Our results support the use of low-energy electron-beam spectroscopies for the exploration of nonlinear optical processes in nanostructures.