Organic−inorganic hybrids may offer material properties not available from their inorganic components. However, they are typically less stable and disordered. Long-term stability study of the hybrid materials, over the anticipated lifespan of a real-world electronic device, is practically nonexistent. Disordering, prevalent in most nanostructure assemblies, is a prominent adversary to quantum coherence. A family of perfectly ordered II−VI-based hybrid nanostructures has been shown to possess many unusual properties and potential applications. Here, using a prototype structure β-ZnTe(en) 0.5 a hybrid superlatticeand applying an array of optical, structural, surface, thermal, and electrical characterization techniques, in conjunction with densityfunctional theory calculations, we have performed a comprehensive and correlative study of the crystalline quality, structural degradation, electronic, optical, and transport properties on samples from over 15 years old to the recently synthesized. The findings show that not only do they exhibit an exceptionally high level of crystallinity in both macroscopic and microscopic scale, comparable to high-quality binary semiconductors; and greatly enhanced material properties, compared to those of the inorganic constituents; but also, some of them over 15 years old remain as good in structure and property as freshly made ones. This study reveals (1) what level of structural perfectness is achievable in a complex organic−inorganic hybrid structure or a man-made superlattice, suggesting a nontraditional strategy to make periodically stacked heterostructures with abrupt interfaces; and (2) how the stability of a hybrid material is affected differently by its intrinsic attributes, primarily formation energy, and continued...

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Organic–inorganic hybrid materials often face a stability challenge. β‐ZnTe(en)0.5, which uniquely has over 15‐year real‐time degradation data, is taken as a prototype structure to demonstrate an accelerated thermal aging method for assessing the intrinsic and ambient‐condition long‐term stability of hybrid materials. Micro‐Raman spectroscopy is used to investigate the thermal degradation of β‐ZnTe(en)0.5 in a protected condition and in air by monitoring the temperature dependences of the intrinsic and degradation‐product Raman modes. First, to understand the intrinsic degradation mechanism, the transition state of the degradation is identified, then using a density functional theory, the intrinsic energy barrier between the transition state and ground state is calculated to be 1.70 eV, in excellent agreement with the measured thermal degradation barrier of 1.62 eV in N2 environment. Second, for the ambient‐condition degradation, a reduced thermal activation barrier of 0.92 eV is obtained due to oxidation, corresponding to a projected ambient half‐life of 40 years at room temperature, in general agreement with the experimental observation of no apparent degradation over 15 years. Furthermore, the study reveals a mechanism, conformation distortion enhanced stability, which plays a pivotal role in forming the high kinetic barrier, contributing greatly to the impressive long‐term stability of β‐ZnTe(en)0.5.