Abstract
The longitudinal static second hyperpolarizability (γ) has been investigated for models (H3 + and H5 +) open-shell singlet one-dimensional systems bearing a charged defect. Using various ab initio molecular orbital and density functional theory methods, the γ values of these cationic symmetric hydrogen chain models having different bond-length alternations (BLAs) are analyzed as a function of the average diradical character as well as by adopting the summation-over-states scheme. These systems exhibit negative γ values, of which the amplitudes increase nonlinearly with the average diradical character while the chain-length dependence is enhanced by increasing the BLAs. This dependence of γ with the diradical character is mostly dictated by the strong decrease of the excitation energies.
Original language | English |
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Pages (from-to) | 111-115 |
Number of pages | 5 |
Journal | Chemical Physics Letters |
Volume | 451 |
Issue number | 1-3 |
DOIs | |
Publication status | Published - 17 Jan 2008 |