Single acquisition reconstruction of nonlinear susceptibility and Raman tensors at the diffraction limit

Raman spectroscopy and Second Harmonic Generation (SHG) are complementary, non-destructive techniques that provide rich and distinct insights into the structural and electronic properties of materials. Raman spectroscopy offers detailed information on vibrational modes, phase transitions, temperature, and local stress, while SHG is highly sensitive to symmetry and orientation, particularly in non-centrosymmetric structures. In this work, in addition to combining both techniques, we propose a novel approach to determine the nonlinear optical tensor, leveraging the spatial and ultra-fast temporal offset of a Bessel-Gaussian laser beam at the microscope’s focal point.