CO₂ Sensing Characteristics of 2H-MoS₂-Coated D-Shaped Optical Fiber Sensors

In this study, a highly crystalline 2H (hexagonal)-phase MoS₂ sensing layer with a precisely controlled crystal structure was realized through a combination of DC sputtering and sulfurization annealing processes, and subsequently integrated with a D-shaped optical fiber to develop a highly sensitive carbon dioxide (CO₂) sensor. Conventionally sputtered MoS₂ thin films often suffer from the presence of unstable metallic 1T (tetragonal) phases and a high density of sulfur vacancies, which significantly degrade sensor reversibility and long-term stability. Here, high-temperature annealing under a sulfur-rich atmosphere was employed to induce a complete phase transition from the metastable 1T phase to the stable semiconducting 2H phase, while simultaneously healing sulfur vacancies. Enhanced crystallinity was confirmed by Raman spectroscopy. The fabricated sensor exhibited excellent linearity (R² > 0.99) and markedly improved repeatability over a CO₂ concentration range of 1000-10,000 ppm. This significant performance enhancement is attributed to reversible charge transfer induced by sulfur vacancy passivation, which modulates the complex refractive index of the MoS₂ layer and optimizes optical interaction with the evanescent field of the D-shaped fiber. The phase engineering and defect-healing strategy presented in this work effectively addresses the drift issues commonly observed in conventional electrical gas sensors and provides a crucial pathway toward the realization of high-performance optical gas sensors.