Calculation of frequency-dependent polarizabilities using the approximate coupled-cluster triples model CC3

Abstract

The calculation of frequency-dependent polarizabilities is discussed for the iterative approximate coupled-cluster singles, doubles and triples model CC3. A new implementation of the linear response functions is reported, which has the same computational O(N7) scaling as CC3 ground state calculations and uses an explicitly spin-coupled excitation space. Sample calculations are presented for the static and frequency-dependent polarizabilities of Ne and ethylene, as well as for the static polarizabilities of HF. The largest calculation employs the t-aug-cc-pVTZ basis set for ethylene giving a total of 328 basis functions. The results obtained agree well with the experimental data.