The mid-infrared (mid-IR) anisotropic optical response of a material probes vibrational fingerprints and absorption bands sensitive to order, structure, and directiondependent stimuli. Such anisotropic properties play a fundamental role in catalysis, optoelectronic, photonic, polymer and biomedical research and applications. Infrared dual-comb polarimetry (IR-DCP) is introduced as a powerful new spectroscopic method for the analysis of complex dielectric functions and anisotropic samples in the mid-IR range. IR-DCP enables novel hyperspectral and time-resolved applications far beyond the technical possibilities of classical Fourier-transform IR approaches.The method unravels structure-spectra relations at high spectral bandwidth up to 90 cm −1 and short integration times of 65 μs, with previously unattainable time resolutions for spectral IR polarimetric measurements for potential studies of noncyclic and irreversible processes. The polarimetric capabilities of IR-DCP are demonstrated by investigating an anisotropic inhomogeneous freestanding nanofiber scaffold for neural tissue applications. Polarization sensitive multi-angle dual-comb transmission amplitude and absolute phase measurements (separately for ss-, pp-, ps-, and sp-polarized light) allow the in-depth probing of the samples' orientation-dependent vibrational absorption properties. Mid-IR anisotropies can quickly be identified by cross-polarized IR-DCP polarimetry.
Key points• A novel dual-comb laser-based technique is established for polarization-dependent mid-infrared spectroscopy.• Independent measurements of spectral s-and p-polarized transmission amplitudes and phases in the μs range.• Visualization of the anisotropy of nanofiber scaffolds as used for neural tissue applications.