Reversible Single‐Pulse Laser‐Induced Phase Change of Sb₂S₃ Thin Films: Multi‐Physics Modeling and Experimental Demonstrations

Abstract Phase change materials (PCMs) have gained a tremendous interest as a means to actively tune nanophotonic devices through the large optical modulation produced by their amorphous to crystalline reversible transition. Recently, materials such as Sb₂S₃ emerged as particularly promising low loss PCMs, with both large refractive index modulations and transparency in the visible and near‐infrared. Controlling the local and reversible phase transition in this material is of major importance for future applications, and an appealing method to do so is to exploit pulsed lasers. Yet, the physics and limits involved in the optical switching of Sb₂S₃ are not yet well understood. Here, the reversible laser‐induced phase transition of Sb₂S₃ is investigated, focusing specifically on the mechanisms that drive the optically induced amorphization, with multi‐physics considerations including the optical and thermal properties of the PCM and its environment. The laser energy threshold for reversibly changing the phase of the PCM is determined through both theoretical analysis and experimental investigation, not only between fully amorphous and crystalline states but also between partially recrystallized states. Then, the non‐negligible impact of the material's polycrystallinity and anisotropy on the power thresholds for optical switching is revealed. Finally, the challenges related to laser amorphization of thick Sb₂S₃ layers are addressed, as well as strategies to overcome them. These results enable a qualitative and quantitative understanding of the physics behind the optically‐induced reversible change of phase in Sb₂S₃ layers.