The molecular configurations and geometric parameters of the carbon chains H-(C≡C) n -H (n = 3-9, 15) have been reported in other literatures . Their response properties in the zero-frequency limit (λ = ∞ nm) and in the frequency-dependent fields (λ = 1907, 1460, 1340, and 1064 nm) calculated by coupled-perturbed Kohn-Sham (CPKS) method are numerically listed in Tables and and graphically shown in Figs. and. For a specific carbon chain, the components of the molecular polarizability in the direction perpendicular to the molecular axis, α xx (λ) and α yy (λ), are significantly smaller than α zz (λ) in the direction of the chain axis, which shows a notable polarization anisotropy and is apparently rationalized by the greater polarization of π-electrons in the axial direction. The components of the molecular polarizability of H-(C≡C) n -H (n = 3-9, 15) increase with the chain length, and the increase of the axial component [α zz (λ)] is the most significant. However, the respective polarizability components of the chains are little influenced by the frequency of the external electric field (EEF), that is, the values of the polarizability calculated at the studied frequency-dependent fields (λ = 1907, 1460, 1340, and 1064 nm) have no obvious change compared to the values in the zero-frequency limit (λ = ∞ nm), which may be common to centrosymmetric molecules with vanishing permanent dipole moments . Due to the centrosymmetric structure of the studied carbon chains, the magnitude of their total first hyperpolarizability is exactly zero and will not be discussed here .