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Laser Induced Periodic Surface Structures Induced by Surface Plasmons Coupled via Roughness

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 Publication date 2013
  fields Physics
and research's language is English




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In this paper the formation mechanisms of the femtosecond laser-induced periodic surface structures (LIPSS) are discussed. One of the most frequently-used theories explains the structures by interference between the incident laser beam and surface plasmon-polariton waves. The latter is most commonly attributed to the coupling of the incident laser light to the surface roughness. We demonstrate that this excitation mechanism of surface plasmons contradicts to the results of laser-ablation experiments. As an alternative approach to the excitation of LIPSS we analyse development of hydrodynamic instabilities in the melt layer.



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We present that surface two-plasmon resonance (STPR) in electron plasma sheet produced by femtosecond laser irradiating metal surface is the self-formation mechanism of periodic subwavelength ripple structures. Peaks of overdense electrons formed by resonant two-plasmon wave pull bound ions out of the metal surface and thus the wave pattern of STPR is carved on the surface by Coulomb ablation (removal) resulting from the strong electrostatic field induced by charge separation. To confirm the STPR model, we have performed analogical carving experiments by two laser beams with perpendicular polarizations. The results explicitly show that two wave patterns of STPR are independently carved on the exposure area of target surface. The time-scale of ablation dynamics and the electron temperature in ultrafast interaction are also verified by time-resolved spectroscopy experiment and numerical simulation, respectively. The present model can self-consistently explain the formation of subwavelength ripple structures even with spatial periods shorter than half of the laser wavelength, shedding light on the understanding of ultrafast laser-solid interaction.
In this Letter we show that the strong coupling between a disordered set of molecular emitters and surface plasmons leads to the formation of spatially coherent hybrid states extended on acroscopic distances. Young type interferometric experiments performed on a system of J-aggregated dyes spread on a silver layer evidence the coherent emission from different molecular emitters separated by several microns. The coherence is absent in systems in the weak coupling regime demonstrating the key role of the hybridization of the molecules with the plasmon.
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.
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