Application of the time-dependent local density approximation to optical activity

As part of a general study of the time-dependent local density approximatio n (TDLDA), we report here calculations of optical activity of chiral molecu les, taking as examples methyloxirane and C-76(-). The theory automatically satisfies sum rules and the Kramers-Kronig relation between circular dichr oism and optical rotatory power. It reproduces the absorption strengths of the strong states quite well and qualitatively describes the chiroptical pr operties; quantitatively, the predictions of the circular dichroism of the lowest states are a factor of 2-4 too high. In the chiral fullerene C-76 th e TDLDA provides a consistent description of the optical absorption spectru m, the circular dichroism spectrum, and the optical rotatory power, except for an overall shift of the theoretical spectrum. [S1050-2947(99)07607-6].