Abstract. Metastable 4-methyl benzophenone (4-MBP, C 14 H 11 O) crystallizes in the polar (pyroelectric) and enantiomorphic space groups (SG) P3 1 and P3 2 . The optical rotation tensor has been measured for 670 nm and the material was tested for evidence of phase-matchability. The absolute structure was determined via three-beam diffraction, showing that the structural right-hand screw 3 1 is combined with positive (right-handed, i.e. clockwise when looking towards the light source) optical rotation, for both tensor components 11 = 22 = 26 (5) o /mm , 33 = 8.3 (5) o /mm (contrary to low-quartz which shows negative optical rotation for 33 and positive rotation for 11 in righthand SP P3 1 2). The non-linear optical tensors for optical rotation, dcoefficients, electro-optic effect and electrogyration have been calculated using a set of electronic polarizabilities as input parameters for a dipole-dipole interaction model that reproduces the experimental refractive indices and optical rotation. Unusually high polarizability volumes are needed for hydrogen atom bonding to aromatic carbons in order to model the optical tensors. However, the non-linear optical coefficients are of average size.