The ability of light to carry and deliver orbital angular momentum (OAM) in the form of optical vortices has attracted much interest. The physical properties of light with a helical wavefront can be confined onto two-dimensional surfaces with subwavelength dimensions in the form of plasmonic vortices, opening avenues for thus far unknown light-matter interactions. Because of their extreme rotational velocity, the ultrafast dynamics of such vortices remained unexplored. Here we show the detailed spatiotemporal evolution of nanovortices using time-resolved two-photon photoemission electron microscopy. We observe both long- and short-range plasmonic vortices confined to deep subwavelength dimensions on the scale of 100 nanometers with nanometer spatial resolution and subfemtosecond time-step resolution. Finally, by measuring the angular velocity of the vortex, we directly extract the OAM magnitude of light.

We demonstrate nanofocusing down to 60 nm with 800-nm light in atomically flat single-crystalline 22-nm-thick gold flakes.

We designed and realized a metasurface (manipulating the local geometry) spiral (manipulating the global geometry) plasmonic lens, which fundamentally overcomes the multiple efficiency and functionality challenges of conventional in-plane plasmonic lenses. The combination of spirality and metasurface achieves much more efficient and uniform linear-polarization-independent plasmonic focusing. As for functionality, under matched circularly polarized illumination the lens directs all of the power coupled to surface plasmon polaritons (SPPs) into the focal spot, while the orthogonal polarization excites only diverging SPPs that do not penetrate the interior of the lens, achieving 2 orders of magnitude intensity contrast throughout the entire area of the lens. This optimal functional focusing is clearly demonstrated by near-field optical microscopy measurements that are in excellent agreement with simulations and are supported by a detailed theoretical interpretation of the underlying mechanisms. Our results advance the field of plasmonics toward functional detection and the employment of SPPs in smart pixels, near-field microscopy, lithography, and particle manipulation.

Transformation of light carrying spin angular momentum (SAM) to optical field vortices carrying orbital angular momentum (OAM) has been of wide interest in recent years. The interactions between two optical fields, each carrying one of those degrees of freedom, and furthermore, the transfer of the resulting angular momentum product to matter are seldom discussed. Here, we measure the interaction between 3D light carrying axial SAM and 2D plasmon-polariton vortices carrying high-order transverse OAM. The interaction is mediated by two-photon absorption within a gold surface, imprinting the resulting angular-momentum mixing into matter by excitation of electrons that are photo-emitted into vacuum. Interestingly, the spatial distribution of the emitted electrons carries the signature of a subtraction of the spin from the orbit angular momenta. We show experimentally and theoretically that the absorptive nature of this interaction leads to both single and double photon-plasmon angular momentum mixing processes by one-and two-photon interactions. Our results demonstrate high order angular momenta light-matter interactions, provide a glimpse into specific electronic excitation routes, and may be applied in future electronic sources and coherent control.

Orbital angular momentum of light is a core feature in photonics. Its confinement to surfaces using plasmonics has unlocked many phenomena and potential applications. Here, we introduce the reflection from structural boundaries as a new degree of freedom to generate and control plasmonic orbital angular momentum. We experimentally demonstrate plasmonic vortex cavities, generating a succession of vortex pulses with increasing topological charge as a function of time. We track the spatiotemporal dynamics of these angularly decelerating plasmon pulse train within the cavities for over 300 femtoseconds using time-resolved photoemission electron microscopy, showing that the angular momentum grows by multiples of the chiral order of the cavity. The introduction of this degree of freedom to tame orbital angular momentum delivered by plasmonic vortices could miniaturize pump probe–like quantum initialization schemes, increase the torque exerted by plasmonic tweezers, and potentially achieve vortex lattice cavities with dynamically evolving topology.