Decoupling Carrier Dynamics and Energy Transport in Ultrafast Near-Field Nanoscopy.

Ultrafast near-field optical nanoscopy has emerged as a powerful platform to characterize low-dimensional materials. While analytical and numerical models have been established to account for photoexcited carrier dynamics, quantitative evaluation of the associated pulsed laser heating remains elusive. Here, we decouple the photocarrier density and temperature increase in near-field nanoscopy by integrating the two-temperature model (TTM) with finite-difference time-domain (FDTD) simulations. These results reveal that the electron-phonon coupling in a silicon film after femtosecond laser excitation is most pronounced within approximately 3 ps─substantially shorter than the photocarrier decay time scale at tens of picoseconds. Moreover, the coupled TTM-FDTD method indicates that ultrafast laser heating can cause up to a 14% variation in the near-field signal at a 220 μJ/cm pump pulse fluence. Our numerical results are further validated by transient experiments, highlighting the potential of this method for investigations of carrier and thermal phenomena in emerging nanomaterials and nanodevices.