When light illuminates the junction formed between a sharp metal tip and a sample, different mechanisms can contribute to the measured photoinduced force simultaneously. Of particular interest are the instantaneous force between 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 2 force mechanisms is their spectral behavior. The magnitude of the thermal response follows a dissipative (absorptive) Lorentzian line shape, 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. Because the 2 interactions are sometimes comparable in magnitude, the origin of the chemical selectivity in nanoscale spectroscopic imaging through force detection is often unclear. Here, we demonstrate theoretically and experimentally how the light illumination gives rise to the 2 kinds of photoinduced forces at the tip-sample junction in the midinfrared. We comprehensively address the origin of the spectroscopic forces by discussing cases where the 2 spectrally dependent forces are entwined. The analysis presented here provides a clear and quantitative interpretation of nanoscale chemical measurements of heterogeneous materials and sheds light on the nature of light-matter coupling in optomechanical force-based spectronanoscopy.

Coherent Raman scattering (CRS) microscopy is gaining acceptance as a valuable addition to the imaging toolset of biological researchers. Optimal use of this label-free imaging technique benefits from a basic understanding of the physical principles and technical merits of the CRS microscope. This tutorial offers qualitative explanations of the principles behind CRS microscopy and provides information about the applicability of this nonlinear optical imaging approach for biological research.

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.

We use a hemispheric sapphire lens in combination with an off-axis parabolic mirror to demonstrate high-resolution vibrationally resonant sum-frequency generation (VR-SFG) microscopy in the mid-infrared range. With the sapphire lens as an immersed solid medium, the numerical aperture (NA) of the parabolic mirror objective is enhanced by a factor of 1.72, from 0.42 to 0.72, close to the theoretical value of 1.76 ( = nsapphire). The measured lateral resolution is as high as 0.64 μm. We show the practical utility of the sapphire immersion lens by imaging collagen-rich tissues with and without the solid immersion lens.