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Abstract Since the first isolation of graphene, the importance of van der Waals (vdW) interactions has become increasingly recognized in the burgeoning field of layered materials. In this work, infrared nanoimaging techniques and theoretical modeling are used to unravel the critical role played by interfacial vdW interactions in governing the stability of violet phosphorus (VP)—a recently rediscovered wide bandgap p‐type semiconductor—when exfoliated on different substrates. It is demonstrated that vdW interactions with the underlying substrate can have a profound influence on the stability of exfoliated VP flakes and investigate how these interactions are affected by flake thickness, substrate properties (e.g., substrate hydrophilicity, surface roughness), and the exfoliation process. These findings highlight the key role played by interfacial vdW interactions in governing the stability and physical properties of layered materials, and can be used to guide substrate selection in the preparation and study of this important class of materials.

Abstract Violet phosphorus (VP) is garnering attention for its appealing physical properties and potential applications in optoelectronics. A comprehensive investigation of the photodegradation and thermal effects of exfoliated VP on SiO2/Si substrates is presented. The degradation rate of VP is strongly influenced by the wavelength and exposure duration of light. Light illumination of VP above the bandgap leads to faster degradation, attributed to interactions with reactive oxygen species. Power‐dependent photoluminescence (PL) measurements at low temperature (T = 4 K) show neutral exciton (X0) and trion (T) intensities linearly increase with excitation power, while the energy difference between peak energies decreases. The T/X0 spectral weight ratio increases from 0.28 at 300 K to 0.69 at 4 K, suggesting enhanced T formation due to reduced phonon scattering. Temperature‐dependent Raman is used to investigate the phonon properties of VP. Tracking peak positions of 9 Raman modes with temperature, the linear first‐order temperature coefficient is obtained and found to be linear for all modes. The results provide a deeper understanding of VP's degradation behavior and implications for optoelectronic applications.