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The properties of chalcogenide phase change materials have long attracted the scientific community due to a combination of state retention (i.e., memory) and a large contrast in electrical and optical properties between different solid phases. The last decade has witnessed a vast interest in utilizing this material family for optics and photonics, given their large refractive index modulation, nonvolatility—elusive in optics—and straightforward integration into photonic devices. Thus, designing new optical phase change materials (O-PCMs) and demonstrating high-performance applications have become fast-growing research topics. However, advances in O-PCMs have predominantly followed empirical device developments, driven by their promise in trending technological applications. Nonetheless, a growing interest in revealing their materials science intricacies is driving the much-needed effort toward a holistic understanding and codesign of O-PCMs, which is required to fill knowledge gaps, expand the materials library, and solve the most pressing device performance challenges.