Second Harmonic Generation Spectroscopy of the Surface Charge Density Wave in the Weyl Semimetal CoSi

Abstract

Using temperature-dependent rotational anisotropy second harmonic generation (RA-SHG), we identify a charge density wave (CDW) instability on the CoSi (001) face with an onset temperature at $90.0 \pm 0.8$ K. The SHG response tracks the order parameter amplitude, dominated by two nonlinear tensor elements, whose background-subtracted intensity evolves with temperature as a power law. The extracted critical exponent $\beta = 0.30 \pm 0.03$ is consistent with the 3D XY universality class, an unexpected result for a nominally two-dimensional surface layer. No corresponding anomaly is observed in the bulk response, establishing the transition as a purely surface-driven phase transition. We attribute this unexpected scaling to the coupling between surface Fermi-arc states and the bulk topology they are tied to, grounded in a previously observed intra-unit-cell phase relationship between surface sublayers that gives the order parameter intrinsic three-dimensional structure.