Enhanced High-Order Harmonic Generation from Ethylbenzene in Circularly Polarized Laser Fields

We theoretically investigate high-order harmonic generation from ethylbenzene (C8H10), toluene (C7H8), and benzene (C6H6) molecules driven by a circularly polarized laser field using time-dependent density functional theory. By comparing the harmonic spectra of these structurally related molecules, we find that ethylbenzene, which features a larger molecular size due to the ethyl group, exhibits a higher harmonic cutoff and stronger harmonic intensity than toluene and benzene. Time-resolved electron density distributions, together with the probability current density analysis, indicate that under long-wavelength conditions (e.g., 1200 nm), the ethyl group in ethylbenzene and the methyl group in toluene significantly enhance the probability of ionized electrons from neighboring nuclei colliding with nearby nuclei, thereby leading to stronger harmonic emission, with ethylbenzene > toluene > benzene. In contrast, under short-wavelength conditions (e.g., 200 nm), the harmonic intensities of the three molecules show little difference, and the effects of the ethyl and methyl groups on the harmonic yield can be neglected. The influence of laser intensity and wavelength on high-order harmonic generation is further analyzed, confirming the robustness of the structural enhancement effect. Additionally, we study the harmonic ellipticity of ethylbenzene under different carrier-envelope phases, and find that while circularly polarized harmonics can be obtained, their spectral continuity is insufficient for synthesizing isolated circularly polarized attosecond pulses. This limitation is attributed to the broken ring symmetry caused by the ethyl substitution. Our findings offer insight into the relationship between molecular structure and harmonic response in strong-field physics, and provide a pathway for designing efficient circularly polarized attosecond pulse sources.