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Dark Plasmon Modes in Symmetric Gold Nanoparticle Dimers Illuminated by Focused Cylindrical Vector Beams
摘要： The plasmon hybridization model of electromagnetic coupling between plasmonic nanoparticles predicts the formation of lower energy “bonding” and higher energy “antibonding” modes in analogy with the quantum mechanical description of chemical bonding. For a symmetric metallic nanoparticle dimer excited by linearly polarized light, the hybridization picture predicts that in-phase coupling of the dipole moments is optically allowed, creating bright “modes”, whereas the out-of-phase coupling is dark due to the cancellation of the oppositely oriented dipole moments (in the quasistatic approximation). These bright modes are electric dipolar in nature and readily couple to scalar (i.e., linearly or circularly polarized) beams of light. We show that focused cylindrical vector beams, specifically azimuthally and radially polarized beams, directly excite dark plasmon modes in symmetric gold nanoparticle (AuNP) dimers at normal incidence. We use single-particle spectroscopy and electrodynamics simulations to study the resonance scattering of AuNP dimers illuminated by azimuthally and radially polarized light. The electric field distributions of the focused azimuthal or radial beams are locally polarized perpendicular or parallel to the AuNP dimer axis, but with opposite directions at each particle. Therefore, the associated combinations of single-particle dipole moments are out-of-phase, and the excitation (resonance) is of so-called “dark modes”. In addition, multipole expansion of the fields associated with each scattering spectrum shows that the vector beam excitation involves driving multipolar, e.g., magnetic dipolar and electric quadrupolar, modes, and that they even dominate the scattering spectra (vs electric dipole). This work opens new opportunities for investigating dark plasmon modes in nanostructures, which are difficult to selectively excite by conventional polarized light.
关键词： electrodynamics simulations,dark plasmon modes,plasmon hybridization,single-particle spectroscopy,gold nanoparticle dimers,cylindrical vector beams
更新于2025-09-23 15:21:21
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Light-Induced Coalescence of Plasmonic Dimers and Clusters
摘要： The properties of nanoplasmonic structures depend strongly on their geometry, creating the need for high-precision control and characterization. Here, by exploiting the low activation energy of gold atoms on nanoparticle surfaces, we show how laser irradiation re-shapes nanoparticle dimers. Time-course dark-field micro-spectroscopy allows this process to be studied in detail for individual nanostructures. Three regimes are identified: facet growth, formation of a conductive bridge between particles, and bridge growth. Electromagnetic simulations confirm the growth dynamics and allow measurement of bridge diameter, found to be highly reproducible and also self-limiting. Correlations in spectral resonances for the initial and final states give insights into the energy barriers for bridge growth. Dark-field microscopy shows that coalescence of multiple gaps in nanoparticle clusters can be digitally triggered, with each gap closing after discrete increases in irradiation power. Such control is important for light-induced nanowire formation or trimming of electronic and optoelectronic devices.
关键词： nanoparticle coalescence,gold nanoparticles,optical spectroscopy,plasmonics,sintering,nanoparticle dimers
更新于2025-09-23 15:19:57
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Reactive optical matter: light-induced motility in electrodynamically asymmetric nanoscale scatterers
摘要： From Newton’s third law, which is known as the principle of actio et reactio, we expect the forces between interacting particles to be equal and opposite for closed systems. Otherwise, “nonreciprocal” forces can arise. This has been shown theoretically in the interaction between dissimilar optically trapped particles that are mediated by an external field. As a result, despite the incident external field not having a transverse component of momentum, the particle pair experiences a force in a direction that is transverse to the light propagation direction. In this letter, we directly measure the net nonreciprocal forces in electrodynamically interacting asymmetric nanoparticle dimers and nanoparticle structures that are illuminated by plane waves and confined to pseudo one-dimensional geometries. We show via electrodynamic theory and simulations that interparticle interactions cause asymmetric scattering from heterodimers. Therefore, forces are actually a consequence of momentum conservation. Our study demonstrates that asymmetric scatterers exhibit directed motion due to the breakdown of mirror symmetry in their electrodynamic interactions with external fields.
关键词： momentum conservation,nonreciprocal forces,optical binding,electrodynamic interactions,nanoparticle dimers
更新于2025-09-09 09:28:46