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Mesoscopic electrodynamics at metal surfaces: - From quantum-corrected hydrodynamics to microscopic surface-response formalism

Synthesis of porous Ag–Ag2S@Ag–Au hybrid nanostructures with broadband absorption properties and their photothermal conversion application

Plasmonic photocatalysis has attracted interest for its potential to generate energy-efficient reactions, but ultrafast internal conversion limits efficient plasmon-based chemistry. Resonance energy transfer (RET) to surface adsorbates offers a way to outcompete internal conversion pathways and also eliminate the need for sacrificial counter-reactions. Herein, we demonstrate RET between methylene blue (MB) and gold nanorods (AuNRs) using in situ single-particle spectroelectrochemistry. During electrochemically driven reversible redox reactions between MB and leucomethylene blue (LMB), we show that the homogeneous line width is broadened when spectral overlap between AuNR scattering and absorption of MB is maximized, indicating RET. Additionally, electrochemical oxidative oligomerization of MB allowed additional dipole coupling to generate RET at lower energies. Time-dependent density functional theory-based simulated absorption provided theoretical insight into the optical properties, as MB molecules were electrochemically oligomerized. Our findings show a mechanism for driving efficient plasmon-assisted processes by RET through the change in the chemical states of surface adsorbates. 

Plasmon Energy Transfer Driven by Electrochemical Tuning of Methylene Blue on Single Gold Nanorods

Heterostructure manufacturing has been extensively studied as indispensable footstones in the progressive semiconductor optoelectronic devices due to their constituent materials, interfacial states and electronic transport capabilities, thus enabling competitive candidates...

Interfacial modulation and plasmonic effect mediated high-brightness green light sources in a single Ga-doped ZnO microwire based heterojunction

Understanding the differences between photon-induced 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-photon-photoemission (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 the one 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 towards high excitation energies and small in-plane momenta, which suggests a fundamentally different mechanism of hot electron generation, as previously unknown for surface plasmons.

Energy and Momentum Distribution of Surface Plasmon-induced Hot Carriers Isolated via Spatiotemporal Separation

The Particle-in-Cell (PIC) method for plasmons provides a mechanical, single-particle picture of plasmon resonances by tracking in time the movement of all the individual conduction electrons. By applying it to gold nanorods, we demonstrate the usefulness of PIC for extracting time-domain information of plasmons such as plasmon decay times, the relative contribution of each plasmon damping channel, detailed electron movement, as well as radiation and hot electron-emission during damping. An analysis of the time-resolved velocity distribution of the conduction electrons shows that only a small offset in this distribution in each cycle constitutes the plasmon oscillation. We show how PIC can be used to separately analyse Landau damping and Drude damping, and how their decay times can be calculated. Electron–electron scattering and surface scattering are both shown to gradually increase the overall kinetic energy of the electrons and decrease their coherence.

Electron dynamics in plasmons.

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Electron dynamics in plasmons.