Size-Dependent High-Order Harmonic Generation from Linear Carbon-Chain Molecules in Linearly Polarized Laser Fields

Abstract:High-order harmonic generation from molecules is highly sensitive to molecular geometry and strong-field electron dynamics, providing a powerful route for probing and controlling ultrafast processes in extended systems. In this work, we systematically investigate the influence of molecular chain length on HHG from linear carbon-chain molecules C$_2$H$_2$, C$_6$H$_2$, and C$_{10}$H$_2$ driven by an 800 nm linearly polarized laser field. To isolate the molecular-size effect from the influence of different ionization potentials, the laser intensities are adjusted to maintain the same Keldysh parameter for different molecules. Real-time time-dependent density functional theory simulations are performed with the molecular axis aligned parallel to the laser polarization direction. The results show that increasing the molecular chain length significantly enhances the harmonic yield and tends to extend the cutoff region. In particular, C$_{10}$H$_2$ exhibits much stronger plateau harmonics than C$_2$H$_2$, while the intermediate molecule C$_6$H$_2$ shows harmonic intensities between those of C$_2$H$_2$ and C$_{10}$H$_2$. Time-frequency analysis and charge-density evolution reveal that the enhanced HHG emission in longer chains originates from the enlarged electron acceleration distance and increased probability of multi-center recollision, especially near the terminal carbon atoms. These findings demonstrate that molecular-size engineering offers an effective strategy for controlling harmonic emission and optimizing attosecond light sources in extended molecular systems.

arXiv:2610.21712 [quant-ph]

(or arXiv:2610.21712v1 [quant-ph] for this version)

https://doi.org/10.48550/arXiv.2610.21712 Focus to learn more arXiv-issued DOI via DataCite (pending registration)

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