TY - JOUR
T1 - An elementary description of nonlinear optical properties of octupolar molecules
T2 - Four-state model for guanidinium-type molecules
AU - Cho, Minhaeng
AU - Kim, Hyun Soo
AU - Jeon, Seung Joon
PY - 1998/5/1
Y1 - 1998/5/1
N2 - A theoretical description of the molecular polarizability (α) and first and second hyperpolarizabilities (β and γ) of a guanidinium-type octupolar molecule is presented. By using a valence bond and three charge-transfer states with nonzero transfer integrals, the electronic states are obtained as linear combinations of these basis states. It is found that a doubly degenerate excited state is only optically coupled to the ground state. Based on the analytic expressions for α, β, and γ obtained, it is shown that the resultant tensor elements of β satisfy the symmetry requirements of point group D3h. Unlike the linear push-pull polyenes, the magnitudes of α, β, and γ of the guanidinium-type octupolar molecules increase as the charge-transfer character of the electronic ground state increases. Also, their dependences on the distance (d) between the donor and acceptor are briefly discussed.
AB - A theoretical description of the molecular polarizability (α) and first and second hyperpolarizabilities (β and γ) of a guanidinium-type octupolar molecule is presented. By using a valence bond and three charge-transfer states with nonzero transfer integrals, the electronic states are obtained as linear combinations of these basis states. It is found that a doubly degenerate excited state is only optically coupled to the ground state. Based on the analytic expressions for α, β, and γ obtained, it is shown that the resultant tensor elements of β satisfy the symmetry requirements of point group D3h. Unlike the linear push-pull polyenes, the magnitudes of α, β, and γ of the guanidinium-type octupolar molecules increase as the charge-transfer character of the electronic ground state increases. Also, their dependences on the distance (d) between the donor and acceptor are briefly discussed.
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U2 - 10.1063/1.476128
DO - 10.1063/1.476128
M3 - Article
AN - SCOPUS:0000731481
VL - 108
SP - 7114
EP - 7120
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
SN - 0021-9606
IS - 17
ER -