Distinguishing local isomorphism classes in quasicrystals by high-order harmonic spectroscopy

Electron diffraction spectroscopy is a fundamental tool for investigating quasicrystal structures, which unveils the quasiperiodic long-range order. Nevertheless, it falls short in effectively distinguishing separate local isomorphism classes. This is a long outstanding problem. Here, we study the high-order harmonic generation in two-dimensional generalized Penrose quasicrystals to optically resolve different local isomorphism classes. The results reveal that: (i) harmonic spectra from different parts of a quasicrystal are identical, even though their atomic arrangements vary significantly. (ii) The harmonic yields of diverse local isomorphism classes exhibit variations, providing a way to distinguish local isomorphism classes. (iii) The rotational symmetry of harmonic yield can serve as a characteristic of quasicrystal harmonics and is consistent with the orientation order. Our results not only pave the way for confirming the experimental reproducibility of quasicrystal harmonics and identifying quasicrystal local isomorphism classes, but also shed light on comprehending electron dynamics influenced by the vertex environments.