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Nanoscale Heat Flow and Thermometry in Laser-Heated Resonant Silicon Mie Nanospheres Probed with Spatially Resolved
Saskia Fiedler1, Loriane Monin1, Hiroshi Sugimoto2
1Department of Sustainable Energy Materials, NWO-Institute AMOLF, Science Park 104, 1098 XG Amsterdam, The Netherlands.
Abstract:
Many nanoscale technologies depend critically on precise knowledge and control of local temperature and heat flow, making robust nanothermometry essential for designing, optimizing, and ensuring the reliability of next-generation devices. In this work, we introduce a correlative method that combines laser excitation with scanning electron microscopy-based cathodoluminescence (SEM-CL) to probe photothermal effects in situ with nanoscale spatial resolution. We analyze the spatially resolved CL (30 keV) of resonant Mie modes in single silicon nanoparticles under continuous-wave laser irradiation (λ = 442 nm). The 235-250-nm-diameter crystalline nanospheres, placed on a Si3N4 membrane, show a strong electric quadrupole CL resonance of which the peak wavelength reversibly red-shifts upon laser-induced heating. A temperature of up to 585 ± 12 °C is derived from the spectral shifts for the highest laser power used (9.6 mW, ∼1 × 106 W/cm2 at the substrate). Numerical heat flow simulations show that the measured steady-state temperatures are consistent with a geometry in which heat flow occurs through a contact area of up to 100 nm2, depending on laser power, between the Si nanosphere and the Si3N4 membrane. We postulate that this contact forms by reshaping of the particle-membrane geometry as it heats up in the initial phase of the laser irradiation, leading to an equilibrium geometry that results in the measured steady-state temperature. This work shows that CL of resonant nanostructures in combination with simulations can serve as sensitive probes of temperature and thermal conductivity. Spatially resolved CL nanothermometry in a SEM enables studies of nanoscale thermal properties of a wide range of device geometries such as electronic integrated circuits, surface catalysts, photovoltaic devices, and more.

