It is worth emphasizing that we are not necessarily advocating for the use of Boys orbitals in TD-DFT, although localized-orbital implementations of TD-DFT have certainly been reported and can be used to reduce cost for large systems, for qualitative analysis, and to eliminate spurious CT states. Similarly, we are not advocating for the use of numerous diffuse shells when one or two is enough to obtain converged properties. That said, Gaussian basis sets with up to n = 8 diffuse shells, 104-107 designed to approximate continuum states, have been used to simulate molecular high-harmonic generation induced by strong laser fields. (Such calculations are typically performed using real-time Kohn-Sham theory. 1 ) Thus, applications of both localized orbitals and ultra-diffuse basis sets do exist in the TD-DFT literature.