Two-dimensional two-photon absorptions and third-order nonlinear optical properties of Ih fullerenes and fullerene onions. Issue 25 (18th June 2020)

• Record Type: Journal Article
• Authors: Zheng, Xue-Lian; Yang, Ling; Shang, Bo; Wang, Ming-Qian; Niu, Yingli; Li, Wei-Qi; Tian, Wei Quan
• Is Part Of: Physical chemistry chemical physics. Volume 22:Issue 25(2020)
• Page Start: 14225
• Page End: 14235
• Publication Date: 2020-06-18
• Subjects: Chemistry, Physical and theoretical -- Periodicals; 541.3
• DOI: 10.1039/d0cp01996h
• Languages: English
• ISSNs: 1463-9076

Abstract

Abstract : The third order nonlinear optical properties of I h symmetry fullerenes increase exponentially with fullerene size. The two-dimensional two-photon absorption spectra for C60 and C240 have strong self-phase modulation responses. Abstract : The third order static and dynamic nonlinear optical (NLO) responses of I h 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 I h symmetry fullerenes increases exponentially with fullerene size [from 10.00 × 10 −34 esu in C60 to 3266.74 × 10 −34 esu ≈ γ 0 (C60 ) × 9 2.63 in C540 ]. The external fields of strong third order NLO responses of I h 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.