Because of its wide utility, polarizability has been the topic of a number of recent computational benchmark studies. Hait and Head-Gordon provided a thorough examination of the performance of a large number of density functional theory (DFT) functionals at the complete basis set (CBS) limit for 132 small molecules. Frediani et. al. used a subset of the Head-Gordon study's molecule set to test the veracity of that study's CBS limit claim using alternative multiwavelet bases in order to reduce potential error. Sauer and co-workers used a benchmark set of 14 heteroaromatic molecules to assess the accuracy of various second-order methods for both static and frequency dependent polarizabilities. Afzal and Hachmann tested various DFT methods to determine the best way to balance accuracy and e ciency for high-throughput non-conjugated polymer screening. 12 While all of these studies provide valuable insight into the relative accuracy of various polarizability methods for di↵erent applications, none of them examine such methods for the high polarizability limit. As shown in our previous work using a genetic algorithm (GA) to search for high dielectric oligomers, there is a need for a polarizability method capable of calculating large polarizabilities (on the scale of 10 2 Å3 ) while making e cient use of time and computational resources. As a point of reference, all of the molecular species examined by the previously mentioned studies possess isotropic polarizabilities less than 40 Å3 .