For the study of attosecond physics and petahertz electronics, it is necessary to measure precisely the optical waveform of short pulses, including the carrier-envelope phase. A promising approach is to use the optical field emission from metal nanostructure, where the electron tunneling from metal surface is driven by plasmonic near fields. However, there have been problems of low current levels and laser-induced damages of metal nanostructures. Here, we develop an all-solid-state optical-field detector based on metal-insulator hybrid nanostructures, which works in the nanojoule range. The photoelectric efficiency is substantially increased because of the lowered energy barrier for photoemission and the higher near-field enhancements originating from the metal-insulator-metal plasmon. Laser-induced damage resistance is also improved by encapsulating the metal nanoantennas with dielectric materials.
We demonstrate that metal-carbonyl compounds in liquid n-hexane are dissociated and adsorbed on gold surfaces upon vibrational excitation. We illuminate gold nanoantennas with temporally-shaped mid-infrared pulses to produce intense plasmonic near-fields. The produced near-fields induce vibrational ladder climbing and the resultant dissociation of metal-carbonyl compounds. A new band, cumulatively increase with irradiation, is attributed to the molecular species which are dissociated and adsorbed on gold surfaces. This demonstration proves that the plasmonic near-fields of midinfrared pulses are useful for mode-selective reaction control at electronic ground states and for possible subsequent manipulation of molecules like trapping and alignment.
Plasmonic enhancements of optical near-fields with metal nanostructures offer extensive potential for amplifying lightmatter
interactions. We analytically formulate the enhancement of linear and nonlinear optical responses of molecular
vibrations through resonant nanoantennas, based on a coupled-dipole model. We apply the formulae to evaluation of
signal enhancement factors in the antenna-enhanced vibrational spectroscopy.
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