2024/09/17 by Stephanie N. Armond, Armond, Stephanie N., Kyle Hamer +11
Biochemistry, Genetics and Molecular Biology · Engineering · Materials Science · #Atomic Physics (physics.atom-ph) #Electron Spin Resonance Studies #FOS: Physical sciences #Organic Light-Emitting Diodes Research #Organic and Molecular Conductors Research
paper · pdf · doi:10.48550/arxiv.2409.11487
openalex publication_date 2024/09/17 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
We compare the high-harmonic-generation (HHG) yield driven by a mid-infrared laser in three organic ring-shaped molecules, calculated using time-dependent density-functional theory (TDDFT). We average the yield over the relative orientation of the molecules and the linearly-polarized, 1825 nm driving laser pulse in order to compare to experimental spectra obtained by Alharbi et al., Phys. Rev. A 92, 041801 (2015). We find that the raw TDDFT-calculated HHG yield in cyclohexane (CHA) is strongly overestimated compared to those of benzene and cyclohexene, and that this can be attributed to unphysically large contributions from CHA orbitals lying well below the highest-occupied molecular orbital. We show that implementing a simple orbital-resolved scaling factor, which corrects the yield of the tunneling ionization contribution to the first step in the HHG process, leads to much better comparisons with experimental results. Our results are encouraging for the use of TDDFT in systematic computations of HHG in large molecules.