Uniaxial Strain Engineering of Anisotropic Phonon in Few‐Layer Violet Phosphorus with High Stretchability for Polarized Sensitive Flexible Photodetector

Abstract The manifestation of mechanical phenomena in quantum materials at the macroscopic level is intricately linked to pronounced electron‐electron interactions within their lattices, a relationship that becomes especially evident in low‐dimensional materials. Violet phosphorous (VP), a nascent 2D material distinguished by its unique vertically aligned tubular structures, has garnered considerable attention owing to its layer‐dependent electronic bandgap, exceptional carrier mobility, and robust air stability. Herein, a comprehensive exploration of the phonon modes exhibited by few‐layer VP through an integrated experimental‐theoretical approach, focusing on the modulation of their Raman response under the uniaxial strain along a ‐axis, b ‐axis, and tube direction, respectively, is undertaken. Density functional theory calculations highlight when strain is applied along the a ‐ or b ‐axis direction, the strain is predominantly mitigated through tube rotational adaptations instead of the change of bond length and bond angle, culminating in a pronounced anisotropic Raman response. Moreover, the strain engineering can effectively optimize the photoelectric response performance of VP, including increase the responsivity ≈2500% and elevate the anisotropic ratio from 2.26 to 3.38. This investigation not only confirms the superior stretchability and impact resistance properties of cross‐structured VP but also establishes the groundwork for exploring the strain‐induced anisotropic optoelectric properties to VP.