ABSTRACT
Active light-emitting all-dielectric nanoantennas recently have demonstrated great potential as highly efficient nanoscale light sources owing to their strong luminescent and Raman responses. However, their large-scale fabrication faces a number of problems related to productivity limits of existing lithography techniques. Thus, high-throughput fabrication strategies allowing in a facile way to tailor of the nanoantenna emission and thermal properties in the process of their fabrication are highly desirable for various applications. Here, we propose a cost-effective approach to large-scale fabrication of Si1-xGex alloyed Mie nanoresonators possessing an enhanced inherent Raman response which can be simply tailored via tuning the Ge concentration. Moreover, by tailoring the relative Ge composition one can gradually change a complex refractive index of the produced Si1-xGex alloy, which affects the ratio between radiative and nonradiative losses in Si1-xGex nanoantennas, which is crucial for optimization of their optical heating efficiency. Composition-tunable Si1-xGex nanoantennas with an optimized size, light-to-heat conversion and Raman response are implemented for non-invasive sensing of 4-aminothiophenol molecules with a temperature feedback modality and high subwavelength spatial resolution. The results are important for advanced multichannel optical sensing, providing information on analyte's composition, analyte-nanoantenna temperature response and spatial position.
ABSTRACT
Hollow reduced-symmetry resonant plasmonic nanostructures possess pronounced tunable optical resonances in the UV-vis-IR range, being a promising platform for advanced nanophotonic devices. However, the present fabrication approaches require several consecutive technological steps to produce such nanostructures, making their large-scale fabrication rather time-consuming and expensive. Here, we report on direct single-step fabrication of large-scale arrays of hollow parabolic- and cone-shaped nanovoids in silver and gold thin films, using single-pulse femtosecond nanoablation at high repetition rates. The lateral and vertical size of such nanovoids was found to be laser energy-tunable. Resonant light scattering from individual nanovoids was observed in the visible spectral range, using dark-field confocal microspectroscopy, with the size-dependent resonant peak positions. These colored geometric resonances in far-field scattering were related to excitation and interference of transverse surface plasmon modes in nanovoid shells. Plasmon-mediated electromagnetic field enhancement near the nanovoids was evaluated via finite-difference time-domain calculations for their model shapes simulated by three-dimensional molecular dynamics, and experimentally verified by means of photoluminescence microscopy and Raman spectroscopy.
