Multi-frequency photothermal interferometry of single aerosol particles

The frequency dependence of photothermal and photoacoustic signals provides information on evaporation, condensation, and heat transfer processes in aerosol particles. Performing such measurements at the single particle level increases accuracy and provides access to various particle properties. Previously, this was not possible due to the resonant acoustic signal amplification required in photoacoustics, which restricted usable modulation frequencies to a single value. In this study, we introduce the use of multi-frequency photothermal interferometry (n$\omega$-PTI) on single, optically trapped particles and experimentally investigate the frequency dependence of the photothermal signal. The observed signal and its dependence on the optical and thermophysical properties of the particle and the interferometer probe beam are analyzed by an accompanying theoretical model. Our measurements prove the applicability of the presented method and indicate a stronger frequency dependence of the photothermal amplitude from single particles than previously observed in bulk measurements. Furthermore, we were able to decouple the contributions from the particle temperature and the thermal wave propagation and examine their frequency dependencies individually. Finally, we analyzed the direct influence of the particle on the measured signal and showed the potential of frequency-resolved photothermal measurements to study thermophysical parameters or optical properties at the single particle level in the Knudsen transition regime.