Nanoscale spectroscopic studies of two different physical origins of the tip-enhanced force: dipole and thermal

Abstract: When light illuminates the junction formed between a sharp metal tip and a sample, different mechanisms can con-tribute to the measured photo-induced force simultaneously. Of particular interest are the instantaneous force be-tween the induced dipoles in the tip and in the sample and the force related to thermal heating of the junction. A key difference between these two force mechanisms is their spectral behaviors. The magnitude of the thermal response follows a dissipative Lorentzian lineshape, which measures the heat exchange between light and matter, while the induced dipole response exhibits a dispersive spectrum and relates to the real part of the material polarizability. Be-cause the two interactions are sometimes comparable in magnitude, the origin of the nanoscale chemical selectivity in the recently developed photo-induced force microscopy (PiFM) is often unclear. Here, we demonstrate theoretically and experimentally how light absorption followed by nanoscale thermal expansion generates a photo-induced force in PiFM. Furthermore, we explain how this thermal force can be distinguished from the induced dipole force by tuning the relaxation time of samples. Our analysis presented here helps the interpretation of nanoscale chemical measure-ments of heterogeneous materials and sheds light on the nature of light-matter coupling in van der Waals materials.