The polarizability and first hyperpolarizability are important response properties of a molecule to an applied electric field, which determine the deformability of charges and the NLO performances of bulk materials, respectively. The unit sphere representation of (hyper)polarizability is a very useful technique for characterizing the (hyper)polarizability tensor of molecules, thereby visualizing anisotropic features of molecular response properties. The (hyper)polarizability density can graphically show the spatial contribution of electrons to the tensorial component of (hyper)polarizability, which is helpful to intuitively understand the essence of the total (hyper)polarizability of molecules. 11,13,14,43,44,50-54 The (hyper)polarizability decomposition can be used to study the (hyper)polarizability values of atoms or groups within molecules, thus quantifying the contribution of specific structural units to the tensorial components of molecular (hyper)polarizability. In the following discussions on the responsive optical properties of C18 and calculated by CPKS method are listed in Table .