Efficient calculation of the rotational g tensor from auxiliary density functional theory.

The computation of the rotational g tensor with the recently developed auxiliary density functional theory (ADFT) gauge including atomic orbital (GIAO) methodology is presented. For the rotational g tensor, the calculation of the magnetizability tensor represents the most demanding computational task. With the ADFT-GIAO methodology, the CPU time for the magnetizability tensor calculation can be dramatically reduced. Therefore, it seems most desirable to employ the ADFT-GIAO methodology also for the computation of the rotational g tensor. In this work, the quality of rotational g tensors obtained with the ADFT-GIAO methodology is compared with available experimental data as well as with other theoretical results at the Hartree-Fock and coupled-cluster level of theory. It is found that the agreement between the ADFT-GIAO results and the experiment is good. Furthermore, we also show that the ADFT-GIAO g tensor calculation is applicable to large systems like carbon nanotube models containing hundreds of atom and thousands of basis functions.