Multiscale simulations of Sb$_2$Te for photonic phase-change applications

Chalcogenide phase-change materials (PCMs) are widely applied in electronic and photonic applications, such as non-volatile memory and neuro-inspired computing. Doped Sb$_2$Te alloys have won the market of rewritable optical discs in the 1990s, and are now gaining increasing attention for on-chip photonic applications, due to their growth-driven crystallization features. However, it remains unknown whether Sb$_2$Te also forms a metastable crystalline phase upon nanoseconds crystallization in devices, similar to the case of nucleation-driven Ge-Sb-Te alloys. Here, we carry out thorough ab initio simulations to understand the structural evolution and changes in optical properties of amorphous Sb$_2$Te upon heating and atomic ordering. We show that the crystallized phase of Sb$_2$Te forms a disordered rhombohedral structure, and additional tellurium ordering reduces the total energy, leading to the ordered rhombohedral ground state. During the continuous transformation process, changes in the dielectric function are highly wavelength-dependent from the visible-light range towards the telecommunication band. Our finite-difference time-domain simulations based on the ab initio input reveal key differences in device output for color display and photonic memory applications upon tellurium ordering, pointing towards different strategies for device programming. Our work serves as an example of how multiscale simulations of materials can guide practical photonic phase-change applications.