Ab initio calculation of nonlinear optical properties for chiral carbon nanotubes. Second harmonic generation and dc-Pockels effect

Michel Rérat (1) , Panaghiotis Karamanis (1) , B. Civalleri (2) , L. Maschio (3) , V. Lacivita , B. Kirtman (4)

1 IPREM - Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux
2 Dipartimento di Chimica IFM and NIS Centre of Excellence
3 Dipartimento di Chimica [Torino]
4 CCS-UCSB - Chemistry and Biochemistry [Santa Barbara]

Although the static first hyperpolarizability β of graphene and chiral carbon nanotubes (CNTs) vanishes by symmetry, that is no longer true for frequency-dependent fields in which case there is a unique nonzero component. We evaluate that component for the dc-Pockels effect and second harmonic generation of several CNTs by means of the coupled perturbed Kohn–Sham method with the CAM-B3LYP functional as implemented in the CRYSTAL code. Both electronic and vibrational contributions are considered. Of particular interest is the frequency dependence in the region below the first resonance. Our results for the role of band gap, type of chirality, CNT radius and effect of orbital relaxation are analyzed using the conventional sum-over-states formulation in conjunction with the calculated band structure and density of states.

Mots clés: Chiral carbon nanotubes; CRYSTAL code; Coupled perturbed Kohn–Sham method; dc-Pockels effect; Second harmonic generation

Domaines: Chimie

Michel Rérat, Panaghiotis Karamanis, B. Civalleri, L. Maschio, V. Lacivita, et al.. Ab initio calculation of nonlinear optical properties for chiral carbon nanotubes. Second harmonic generation and dc-Pockels effect. Theoretical Chemistry Accounts: Theory, Computation, and Modeling, 2018, 137 (2), pp.1-15. ⟨10.1007/s00214-017-2187-7⟩. ⟨hal-01689447⟩