Atmosphere-controlled thermal processing enables tunable optical properties via iron-oxide phase engineering in natural silicate materials

Controlled-atmosphere thermal processing was investigated as a method to engineer iron-oxide phase assemblages in iron-bearing silicate materials. Natural sandstone was heated between 200 and 1000 °C under air, N 2 and CO 2 atmospheres to evaluate how oxygen partial pressure governs redox transformations and the resulting macroscopic optical behaviour. The treatments produced a wide and reproducible range of optical responses from a single starting material. Colour evolution, quantified in the CIELAB space, correlates with bulk mineral transformations. Oxidizing conditions stabilize hematite-dominated assemblages and generate red hues, whereas reduced-oxygen atmospheres promote magnetite formation and progressive darkening. Rock-magnetic measurements identify atmosphere-dependent phase assemblages, including a high-coercivity iron oxide under strongly oxidizing conditions. The magnetic response mirrors the optical evolution, indicating that colour development originates from internal phase transformations. Compressive strength remained within the same order of magnitude as the untreated material across the studied conditions, indicating no catastrophic mechanical degradation. These results show that oxygen availability acts as a key processing variable controlling iron-oxide stability and optical response. The study establishes a process-based approach for tuning optical properties in mineral materials through atmosphere-controlled thermal processing without chemical additives. Unlike previous studies focused on temperature-driven effects or isolated observations, this work demonstrates a reproducible process-based approach to tune optical properties in natural silicate materials through controlled atmosphere engineering.