Discerning Black Phosphorus Crystal Orientation and Anisotropy by Polarized Reflectance Measurement.

Strong in-plane anisotropy of atomic layer and thin-film black phosphorus (P) offers new device perspectives and stimulates increasing interest and explorations, where precisely determining the black P crystal orientation and anisotropic axes is a necessity. Here, we demonstrate that the crystal orientation and intrinsic in-plane optical anisotropy of black P crystals in a broad thickness range (from ∼5 to ∼300 nm) can be directly and precisely determined, by polarized reflectance measurement alone, in visible range. Combining experiments with modeling of optical anisotropy and multilayer interference effects, we elucidate the underlying principles and validate these measurements. The polarized reflectance method is not only easy to implement but also deterministic, nondestructive, and effective for both on-substrate and suspended black P atomic layers and thin films.