Theoretical Study on the Correlation between Open-Shell Electronic Structures and Third-Order Nonlinear Optical Properties in One-Dimensional Chains of π-Radicals.

This paper theoretically investigated the correlation between the open-shell electronic structure and third-order nonlinear optical (NLO) properties of one-dimensional (1D) stacked chains of π-radicals. By employing the finite -mer models consisting of methyl or phenalenyl radicals with different stacking distances, we evaluated the average and standard deviation of diradical characters for -mer models of π-radicals ( and ). Then, we estimated these diradical characters at the limit of → ∞.