Photo-thermo-optical modulation of Raman scattering from Mie-resonant silicon nanostructures

Abstract

Abstract Raman scattering is sensitive to local temperature and thus offers a convenient tool for non-contact and non-destructive optical thermometry at the nanoscale. In turn, all-dielectric nanostructures, such as silicon particles, exhibit strongly enhanced photothermal heating due to Mie resonances, which leads to the strong modulation of elastic Rayleigh scattering intensity through subsequent thermo-optical effects. However, the influence of the complex photo-thermo-optical effect on inelastic Raman scattering has yet to be explored for resonant dielectric nanostructures. In this work, we experimentally demonstrate that the strong photo-thermo-optical interaction results in the nonlinear dependence of the Raman scattering signal intensity from a crystalline silicon nanoparticle via the thermal reconfiguration of the resonant response. Our results reveal a crucial role of the Mie resonance spectral sensitivity to temperature, which modifies not only the conversion of the incident light into heat but also Raman scattering efficiency. The developed comprehensive model provides the mechanism for thermal modulation of Raman scattering, shedding light on the photon–phonon interaction physics of resonant material, which is essential for the validation of Raman nanothermometry in resonant silicon structures under a strong laser field.