Two-dimensional two-photon absorptions and third-order nonlinear optical properties of Ih fullerenes and fullerene onions

Xue-Lian Zheng; Ling Yang; Bo Shang; Ming-Qian Wang; Yingli Niu; Wei-Qi Li; Wei Quan Tian

doi:10.1039/d0cp01996h

Two-dimensional two-photon absorptions and third-order nonlinear optical properties of I_h fullerenes and fullerene onions

Phys Chem Chem Phys. 2020 Jul 1;22(25):14225-14235. doi: 10.1039/d0cp01996h.

Authors

Xue-Lian Zheng¹, Ling Yang², Bo Shang¹, Ming-Qian Wang², Yingli Niu³, Wei-Qi Li⁴, Wei Quan Tian¹

Affiliations

¹ Chongqing Key Laboratory of Theoretical and Computational Chemistry, College of Chemistry and Chemical Engineering, Chongqing University, Huxi Campus, Chongqing 401331, China. tianwq@cqu.edu.cn.
² MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, Institute of Theoretical and Simulational Chemistry, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China.
³ School of Science, Beijing Jiaotong University, Beijing 100044, China. ylniu@bjtu.edu.cn.
⁴ School of Physics, Harbin Institute of Technology, Harbin 150001, China. tccliweiqi@hit.edu.cn and Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan 030006, China.

PMID: 32555864
DOI: 10.1039/d0cp01996h

Abstract

The third order static and dynamic nonlinear optical (NLO) responses of Ih symmetry fullerenes (C60, C240, and C540) and fullerene onions (C60@C240 and C60@C240@C540) are predicted using the ZINDO method and the sum-over-states model. The static second hyperpolarizability of Ih symmetry fullerenes increases exponentially with fullerene size [from 10.00 × 10-34 esu in C60 to 3266.74 × 10-34 esu ≈ γ0(C60) × 92.63 in C540]. The external fields of strong third order NLO responses of Ih symmetry fullerenes change from ultra-violet (C60) to the visible region (C540) as the fullerene size increases. The outer layer fullerene in the fullerene onions has dominant contributions to the third order NLO properties of the fullerene onions, and the inter-shell charge-transfer excitations have conspicuous contributions to the third order NLO properties. The two-dimensional two-photon absorption spectra of C60 and C240 show that those fullerenes have strong two-photon absorptions in the visible region with short wavelength and in the ultra-violet region.