Three-dimensional imaging of ferroaxial domains using circularly polarized second harmonic generation microscopy

The spontaneous symmetry breakdown of matter is one of the most important concepts in materials physics and leads to a phase transition into an ordered phase and domain formation in its consequence. The so-called ‘ferroaxial order’ characterized by a rotational structural distortion with an axial vector symmetry has gained growing interest as a new class of ordered state. However, the observation of ferroaxial domain states, that is, clockwise and counterclockwise rotational states, is not straightforward and has been little investigated. Here, we propose that the circular intensity difference in second harmonic generation (CID-SHG) offers an experimental technique to investigate ferroaxial order and its domain states through the transition process of higher-order multipoles such as magnetic-dipole and electric-quadrupole. By using CID-SHG microscopy, we successfully visualize three-dimensional images of ferroaxial domain structures in NiTiO3. Our results indicate that CID-SHG is a sensitive probe of ferroaxial order and opens possibilities for the use of ferroaxial materials in nonlinear optical manipulations.