Universal visualization of crystalline orientation for black phosphorus by angle-resolved polarized photoacoustic microscopy

Anisotropic two-dimensional (2D) materials, such as black phosphorus (BP), normally possess unique directional in-plane electrical, optical, and thermal properties that are highly correlated with their crystalline orientations. Nondestructive visualization of their crystalline orientation is an indispensable premise for the 2D materials to harness their distinctive strengths in optoelectronic and thermoelectric applications. Here, by photoacoustically recording the anisotropic optical absorption variation under linearly polarized laser beams, an angle-resolved polarized photoacoustic microscopy (AnR-PPAM) is developed, capable of non-invasively determining and visualizing BP's crystalline orientation. We theoretically deduced the physical relationship between the crystalline orientation and polarized photoacoustic (PA) signals, and experimentally proved the ability of AnR-PPAM to universally visualize BP's crystalline orientation regardless of its thickness, substrate, and encapsulation layer. This method provides a new, to the best of our knowledge, strategy for crystalline orientation recognition of 2D materials with flexible measurement conditions, prefiguring important potential for the applications of anisotropic 2D materials.