Descriptors Assisted in Design High-performance Nonlinear Optical Materials with Donor-Acceptor Framework Systems

Abstract

Descriptors can accelerate the search for high-performance nonlinear optical (NLO) materials. Herein, we constructed 48 donor-acceptor (D-A) skeleton systems based on intramolecular B-locking strategies involving TPA-TCN, TPA-CN-N4, and TPA-CN-N4-2Py. The calculated results demonstrated that the constructed D-A molecules can serve as potential NLO material candidates, and torsion angles between donor and acceptor units are concentrated in narrow ranges is beneficial to obtain the large first hyperpolarizability (β). Intriguingly, the desirable R² reached to 0.95 for the TPA-TCN series, 0.96 for the TPA-CN-N4 series and 0.96 for the TPA-CN-N4-2Py series when torsion angles were served as features. Furthermore, when charge transfer and the excited energy of crucial states are used as features, several comprehensive descriptors have been also identified. And the favorable R² values of 0.95 for the TPA-TCN series, 0.97 for the TPA-CN-N4 series, and 0.93 for the TPA-CN-N4-2Py series were achieved between these parameters and lgβ values. These high R² values confirm that these parameters can be regarded as valuable features connecting them to β, aiding in the design of NLO materials with D-A architecture systems. Consequently, these findings provide novel insights into the relationships among torsion angles and β, which facilitates effort to identify high-performance NLO materials within D-A backbone systems tailored for specific application requirements.

Keywords

Donor-acceptor / Torsion angle / Nonlinear optical material / First hyperpolarizability

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Jilin University, The Editorial Department of Chemical Research in Chinese Universities and Springer-Verlag GmbH