Nonlinear Optical Response of a Plasmonic Nanoantenna to Circularly Polarized Light: Rotation of Multipolar Charge Density and Near-Field Spin Angular Momentum Inversion

The spin and orbital angular momentum carried by electromagnetic pulses open new perspectives to control nonlinear processes in light–matter interactions, with a wealth of potential applications. In this work, we use time-dependent density functional theory (TDDFT) to study the nonlinear optical res...

Descripción completa

Detalles Bibliográficos
Autores: Quijada Van den Berghe, Marina, Babaze Aizpurua, Antton, Aizpurua Iriazabal, Francisco Javier, Borisov, Andrei G.
Tipo de recurso: artículo
Fecha de publicación:2023
País:España
Institución:Universidad del País Vasco
Repositorio:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/63834
Acceso en línea:http://hdl.handle.net/10810/63834
Access Level:acceso abierto
Palabra clave:nonlinear optics
light polarization
circularly polarized light
high-harmonic generation
plasmonic nanostructure
time-dependent density functional theory
Descripción
Sumario:The spin and orbital angular momentum carried by electromagnetic pulses open new perspectives to control nonlinear processes in light–matter interactions, with a wealth of potential applications. In this work, we use time-dependent density functional theory (TDDFT) to study the nonlinear optical response of a free-electron plasmonic nanowire to an intense, circularly polarized electromagnetic pulse. In contrast to the well-studied case of the linear polarization, we find that the nth harmonic optical response to circularly polarized light is determined by the multipole moment of order n of the induced nonlinear charge density that rotates around the nanowire axis at the fundamental frequency. As a consequence, the frequency conversion in the far field is suppressed, whereas electric near fields at all harmonic frequencies are induced in the proximity of the nanowire surface. These near fields are circularly polarized with handedness opposite to that of the incident pulse, thus producing an inversion of the spin angular momentum. An analytical approach based on general symmetry constraints nicely explains our numerical findings and allows for generalization of the TDDFT results. This work thus offers new insights into nonlinear optical processes in nanoscale plasmonic nanostructures that allow for the manipulation of the angular momentum of light at harmonic frequencies.