2023/12/01 by Aleksander P. Woźniak, Woźniak, Aleksander P., Robert Moszyński +1 · 1 citation
Physics and Astronomy · Chemistry · #Spectroscopy and Quantum Chemical Studies #Laser-Matter Interactions and Applications #Photochemistry and Electron Transfer Studies
paper · pdf · doi:10.48550/arxiv.2312.00888
We report calculations of the high harmonic generation spectra of the C\textsubscript60 fullerene molecule, employing a diverse set of real-time time-dependent quantum chemical methods. All methodologies involve expanding the propagated electronic wavefunction in bases consisting of the ground and singly excited time-independent eigenstates obtained through the solution of the corresponding linear-response equations. We identify the correlation and exchange effect in the spectra by comparing the results from methods relying on the Hartree-Fock reference determinant with those obtained using approaches based on the density functional theory with different exchange-correlation functionals. The effect of the full random phase approximation treatment of the excited electronic states is also analyzed and compared with the configuration interaction singles and the Tamm-Dancoff approximation. We also showcase that the real-time extension of the semiempirical method INDO/S can be effectively applied for an approximate description of laser-driven dynamics in large systems.