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Understanding the mechanisms and spatial correlations of crystallographicsymmetry breaking in ferroelectric materials is essential to tuning theirfunctional properties. While optical second harmonic generation (SHG) has longbeen utilized in ferroelectric studies, its capability for probing complexpolar materials has yet to be fully realized. Here, we develop a SHG spectralimaging method implemented on a home-designed laser-scanning SHG microscope,and demonstrate its application for a model system of (K,Na)NbO3 singlecrystals. Supervised model fitting analysis produces comprehensive informationabout the polarization vector orientations and relative fractions ofconstituent domain variants as well as their thermal evolution across thepolymorphic phase transitions. We observe an unexpected persistence of theorthorhombic phase at low temperatures, pointing to the phase competitions.Besides, we show that unsupervised matrix decomposition analysis can quicklyand faithfully reveal domain configurations without a priori knowledge aboutspecific material systems. The SHG spectral imaging method can be readilyextended to other ferroelectric materials with potentials to be furtherenhanced.

Delineating complex ferroelectric domain structures via second harmonic generation spectral imaging