Nuclear quantum effects (NQEs) significantly influence many fundamental physical and chemical phenomena. However, their impact on ultrafast dynamics remains poorly understood. Here, we demonstrate that solid-state high-harmonic generation (HHG) provides a promising platform for probing NQEs in attosecond processes. In particular, NQEs substantially modify HHG trajectories due to charge density ripples (CDR) induced by nuclear quantum delocalization. Incorporating NQE-modulated CDR shifts the oscillation phase of HHG, and thus introduces special properties and measurable signatures in the harmonic features, including the emission symmetry and rotation angle of the harmonic polarization ellipse, providing a plausible explanation for recent experimental observations. These findings enable all-optical detection of NQE-driven charge fluctuations via HHG spectroscopy.

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• High-order harmonic generation
• First-principles calculations