Determining the optical and electronic properties of strongly anisotropic materials with symmetries below orthorhombic remains challenging; generalized ellipsometry is a powerful technique in this regard. Here, we employ Mueller matrix spectroscopic and temperature-dependent ellipsometry to determine the frequency dependence of six components of the dielectric-function tensor of the two-dimensional charge-transfer salt -(BEDT-TTF)I across its metal-insulator transition. Our results offer valuable insights into temperature-dependent changes of the components of the spectroscopic dielectric-function tensor across the metal-insulator transition. This advanced method allows extension to other electronic transitions.

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