ABSTRACT
Integrated electronics, photonics and optoelectronics need full control of lattice reconstruction processes in silicon nanostructures at the nanoscale level. However, conventional thermal treatments do not meet the challenging requirements necessary for developing next-generation devices. Light can be a powerful tool to trigger and control opto-thermal effects in resonant nanostructures. Here we propose a new computational approach to light-matter interactions in silicon nanopillars, which simulates heat generation and propagation dynamics occurring in continuous wave laser processing over a wide temporal range (from 1 fs to about 25 hours). We demonstrate that a rational design of the nanostructure aspect ratio, type of substrate, laser irradiation time and wavelength enables amorphous-to-crystalline transformations to take place with a precise, sub-wavelength spatial localization. In particular, we show that visible light can be exploited to selectively crystallize the internal region of the pillars, which is not possible by conventional treatments. A detailed study on lattice crystallization and reconstruction dynamics reveals that local heating drives the formation of secondary antennas embedded into the pillars, highlighting the importance of taking into account the spatial and temporal evolution of the optical properties of the material under irradiation. This approach can be easily extended to many types of nanostructured materials and interfaces, offering a unique computational tool for many applications involving opto-thermal processes (fabrication, data storage, sensing, catalysis, resonant laser printing, opto-thermal therapy, etc. ).
ABSTRACT
Light-to-heat conversion in non-plasmonic, high refractive index nanoantennas is a key topic for many applications, including Raman sensing, laser writing, nanofabrication and photo-thermal therapy. However, heat generation and propagation in non-plasmonic antennas is increasingly debated and contradictory results have been reported so far. Here we report a finite element analysis of the steady-state temperature distribution and heat flow in SiO2/Si core/shell systems (silicon nanoshells) irradiated with different continuous wave lasers (λ = 532, 633 and 785 nm), under real working conditions. The complex interplay among the optical properties, morphology, degree of crystallinity of the nanoshells, thickness dependence of thermal conductivity and interactions with the substrate has been elucidated. This study reveals that all of these parameters can be appropriately combined for obtaining either stable nanoshells for Raman sensing or highly efficient sources of local heating. The optimal balance between thermal stability and field enhancement was found for crystalline Si shell layers with thicknesses ranging from 40 to 60 nm, irradiated by a NIR laser source. On the other hand, non-conformal amorphous or crystalline shell layers with a thickness >50 nm can reach a very high local temperature (above 1000 K) when irradiated with a low power density (less than 1 mW µm-2) laser sources. This work provides a general approach for an extensive investigation of the opto-thermal properties of high-index nanoantennas.
ABSTRACT
Silicon is one of the most interesting candidates for plasmon-free surface-enhaced Raman scattering (SERS), because of its high-refractive index and thermal stability. However, here we demonstrate that the alleged thermal stability of silicon nanoshells irradiated by conventional Raman laser cannot be taken for granted. We investigated the opto-thermal behavior of SiO2/Si core/shell microbeads (Si-rex) irradiated with three common Raman laser sources (λ = 532, 633, 785 nm) under real working conditions. We obtained an experimental proof of the critical role played by bead size and aggregation in heat and light management, demonstrating that, in the case of strong opto-thermal coupling, the temperature can exceed that of the melting points of both core and shell components. In addition, we also show that weakly coupled beads can be utilized as stable substrates for plasmon-free SERS experiments.
