![]() Two-dimensional materials exhibit distinctive electronic properties compared to the bulk that could significantly modify the HHG process, including different symmetries, access to individual valleys and enhanced many-body interactions. The generation process has been discussed in the context of strongly driven electron dynamics in single-particle bands. High-harmonic generation (HHG) in bulk solids permits the exploration of materials in a new regime of strong fields and attosecond timescales. Our study unleashes the power of HHG as a structural characterization tool for technologically important = , The results are generic and are not affected by the Berry curvature, the interband or intraband contribution. This finally links the laser helicity to the crystal structure. It is the circularly polarized laser field that is capable of producing four distinctive HHG signals from the four phases of MoS 2. In this work, we show that a linearly polarized laser pulse used in experiments is not ideal for structural characterization because it only generates in-plane anisotropy. Here, we establish a crucial connection between the symmetry of a material and the helicity of light. High harmonic generation (HHG) emerges as a new frontier that touches the heart of condensed-matter physics from the symmetry to quantum geometrical nature of electrons, but its capability in structural characterization has not been materialized. ![]() Structural characterization is essential to material engineering, but few tools can detect structural properties in the time domain.
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