Facially Polarized Molecule for Alkalides and Superalkalides with Considerable Nonlinear Optical Response

Abstract

AbstractIn this work, alkali M (Li and K) and superalkali M′3O (M′=Li and Na) combined with facially polarized molecule, all‐cis 1,2,3,4,5,6‐Hexafluorocyclohexane (L, C6H6F6), were utilized to design novel alkalides L‐M‐L‐M′ and superalkalides L‐M‐L‐M′3O, respectively. Computational results show that alkalides L‐M‐L‐M′ and superalkalides L‐M‐L‐M′3O have high thermodynamic stability, and the superalkalides L‐M‐L‐M′3O are more stable than the alkalides L‐M‐L‐M′. Importantly, they also possess remarkable NLO responses, the electronic contribution of the static first hyperpolarizability (β0e) has upped to 3.42×106 (a.u.) for L‐K‐L‐Li3O. In particularly, the number of ligand L considerably impacts on β0e value, namely, the β0e value of Li‐L‐Li3O can be improved two orders of magnitude by adding additional ligand L, 1.31×106 (a.u.)(L‐Li‐L‐Li3O) > 7.76×104 (a.u.)(Li‐L‐Li3O). We hope this work can attract researchers to design and synthesize novel excess electron compounds with high performance NLO materials.