We compare the decay of plasmons and “conventional” hot electrons within the same series of gold/metal oxide interfaces. We found an accelerated decay of hot electrons at gold-metal oxide interfaces with decreasing band gap of the oxide material. The decay is accelerated by the increased phase space for electron scattering caused by additional interfacial states. Since plasmons decay faster within the same series of gold-metal oxide interfaces, we propose plasmons are able to decay into the same interfacial states as hot electrons. The similarity of plasmon damping to conventional hot electron decay implies that many classical surface analysis techniques and theoretical concepts are transferable to plasmonic systems. Our results support the mechanism of direct decay of plasmons into interfacial hot electron pairs but the utility of these interfacial states for charge transfer reactions remains to be investigated.
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.
Surface plasmon polaritons carrying orbital angular momentum are of great fundamental and applied interest. However, common approaches for their generation are restricted to having a weak dependence on the properties of the plasmon-generating illumination, providing a limited degree of control over the amount of delivered orbital angular momentum. Here we experimentally show that by tailoring local and global geometries of vortex generators, a change in circular polarization handedness of light imposes arbitrary large switching in the delivered plasmonic angular momentum. Using time-resolved photoemission electron microscopy we demonstrate pristine control over the generation and rotation direction of high-order plasmonic vortices. We generalize our approach to create complex topological fields and exemplify it by studying and controlling a "bright vortex", exhibiting the breakdown of a high-order vortex into a mosaic of unity-order vortices while maintaining the overall angular momentum density. Our results provide tools for plasmonic manipulation and could be utilized in lab-on-a-chip devices. Main:Surface Plasmon Polaritons (SPPs) are evanescent electromagnetic waves propagating along metaldielectric interfaces. In recent years, their ability to carry surface-confined orbital angular momentum (OAM) and form plasmonic vortices has been of wide interest [1][2][3][4][5][6][7]. Understanding and controlling such vortices opens the door towards a variety of applications. Examples are the unlocking of forbidden multipolar transitions in novel light-matter interactions [8-10] and plasmonic tweezers for biological and chemical purposes [11][12][13][14]. For the latter, the trapping and rotating of both dielectric [13] and metallic [11,12,14] microparticles have been demonstrated. For the manipulation of metallic particles,
Understanding the differences between photoninduced and plasmon-induced hot electrons is essential for the construction of devices for plasmonic energy conversion. The mechanism of the plasmonic enhancement in photochemistry, photocatalysis, and light-harvesting and especially the role of hot carriers is still heavily discussed. The question remains, if plasmon-induced and photon-induced hot carriers are fundamentally different or if plasmonic enhancement is only an effect of field concentration producing these carriers in greater numbers. For the bulk plasmon resonance, a fundamental difference is known, yet for the technologically important surface plasmons, this is far from being settled. The direct imaging of surface plasmon-induced hot carriers could provide essential insight, but the separation of the influence of driving laser, field-enhancement, and fundamental plasmon decay has proven to be difficult. Here, we present an approach using a two-color femtosecond pump−probe scheme in time-resolved 2-photonphotoemission (tr-2PPE), supported by a theoretical analysis of the light and plasmon energy flow. We separate the energy and momentum distribution of the plasmon-induced hot electrons from that of photoexcited electrons by following the spatial evolution of photoemitted electrons with energy-resolved photoemission electron microscopy (PEEM) and momentum microscopy during the propagation of a surface plasmon polariton (SPP) pulse along a gold surface. With this scheme, we realize a direct experimental access to plasmon-induced hot electrons. We find a plasmonic enhancement toward high excitation energies and small in-plane momenta, which suggests a fundamentally different mechanism of hot electron generation, as previously unknown for surface plasmons.
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