Face specific doping of Janus all-cis-1,2,3,4,5,6-hexafluorocyclohexane with superalkalis and alkaline earth metals leads to enhanced static and dynamic NLO responses

The first synthesis of all-cis-1,2,3,4,5,6-hexafluorocyclohexane (C6H6F6 = 1), a facially polarized molecule, opened up new avenues for designing novel nonlinear optical (NLO) materials. In the present work, face specific superalkali based alkaline earthides M3O+-1-M - (M = Li,Na,K & M' = Be,Mg,Ca) have been designed theoretically. The NBO analysis and HOMOs electron density confirmed their alkaline earthide nature. The thermodynamic stability was confirmed by their interaction energies (-16.11 to -115.51 kcal/mol). Non-covalent interactions were confirmed through NCI and QTAIM analyses. The maximum absorption in UV-VIS-NIR region confirmed that the complexes are deep UV transparent. The maximum first and second hyperpolarizabilities of 5.2 x 10(6) au and 5.7 x 10(8) au confirmed their enhanced NLO response. The maximum SHG, EOPE and hyper-Rayleigh scattering coefficient (beta(HRS)) are 1.41 x 10(7) au, 3.13 x 10(6) au and 2.1 x 10(6) au, respectively. The EFISHG and EOKE at 4.17 x 10(11) au and 1.51 x 10(11) au have been obtained. The results of quadratic nonlinear refractive index up to 2.16 x 10(-7) au indicated their increased NLO response. These results suggest that designed complexes provide a new insight towards the rational design of stable high performance NLO materials.

Automated summary

The study designed a series of alkaline earthide compounds based on superalkali metals, confirming their alkaline earthide nature and thermodynamic stability, which is significant for enhancing the nonlinear optical response.