Physical mechanism on linear spectrum and nonlinear spectrum in double helical carbon nanomolecule–infinitene

In this work, based on density functional theory (DFT) and wave function analysis, the properties of absorption spectrum, electronic circular dichroism (ECD) spectrum and Raman spectrum of infinitene (monomer and dimer) with double helical structure are theoretically studied. The electronic excitation properties of infinitene were investigated based on the visualization method charge density difference (CDD) and transition density matrix (TDM). It is found that there is obvious intermolecular charge transfer behavior in the dimer. The electromagnetic interaction mechanism of the chirality of infinitene is explained by decomposing transition electric\magnetic dipole moments (TEDMs\TMDMs). The response of Raman spectra to excitation light of different wavelengths was calculated. Then, the electron delocalization degree and magnetic response intensity of infinitene were studied based on the magnetically induced current under external magnetic field. The interaction of infinitene with the external environment was studied by electrostatic and van der Waals potentials, and it was shown that non-polar or low-polar molecules are more inclined to be adsorbed at the groove position of infinitene. Finally, the mechanism of intermolecular interactions in dimer was investigated based on independent gradient model based on Hirshfeld partition (IMGH), Atoms-In-Molecules (AIM), and energy decomposition analysis based on forcefield (EDA-FF). And revealed that the stacking in the dimer is dominated by dispersive interactions.