Abstract
Recent experimental studies highlighted the potential of thin-film crystalline silicon (Si) for high-efficiency solar cells. Using density functional theory, we investigated 2D Si thin films across various orientations, thicknesses, and surface structures to elucidate their structure–property relationships. Through surface-energy calculations and Wulff construction, we determined the crystal habit of Si, which aligns with available experimental observations. Electronic-structure calculations underscored the critical role of valence saturation on surfaces in enabling semiconducting behavior in Si thin films, essential for optical applications. From optical-absorption calculations, we identified the surface index exhibiting the highest absorption coefficients for thin films Si solar cell applications.
