RESUMEN
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 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.
RESUMEN
In this work, we performed an experimental investigation supported by a theoretical analysis, to improve knowledge on the laser ablation of silicon with THz bursts of femtosecond laser pulses. Laser ablated craters have been created using 200 fs pulses at a wavelength of 1030 nm on silicon samples systematically varying the burst features and comparing to the normal pulse mode (NPM). Using bursts in general allowed reducing the thermal load to the material, however, at the expense of the ablation rate. The higher the number of pulses in the bursts and the lower the intra-burst frequency, the lower is the specific ablation rate. However, bursts at 2 THz led to a higher specific ablation rate compared to NPM, in a narrow window of parameters. Theoretical investigations based on the numerical solution of the density-dependent two temperature model revealed that lower lattice temperatures are reached with more pulses and lower intra-burst frequencies, thus supporting the experimental evidence of the lower thermal load in burst mode (BM). This is ascribed to the weaker transient drop of reflectivity, which suggests that with bursts less energy is transferred from the laser to the material. This also explains the trends of the specific ablation rates. Moreover, we found that two-photon absorption plays a fundamental role during BM processing in the THz frequency range.