Abstract Elemental antimony (Sb) is a promising material for phase‐change memory, neuromorphic computing, and nanophotonic applications, because its compositional simplicity prevents phase segregation upon extensive programming. Scaling down the film thickness is a necessary step to prolong the amorphous‐state lifetime. However, the optical properties of Sb are significantly altered as the thickness is reduced to a few nanometers, adding complexity to device optimization. In this work, an atomistic understanding of the thickness‐dependent optical responses is provided in Sb thin films. As thickness decreases, both the extinction coefficient and optical contrast are reduced in the near‐infrared spectrum, consistent with previous optical measurements. Such thickness dependence establishes a practical thickness limit of 2 nm, as predicted by coarse‐grained device simulations. Bonding analysis reveals a fundamentally different behavior for amorphous and crystalline Sb upon downscaling, resulting in the reduction of optical contrast. Thin film experiments are also carried out to validate our predictions. The thickness‐dependent optical trend is demonstrated by ellipsometric spectroscopy experiments, and the bottom thickness limit of 2 nm is confirmed by structural characterization experiments. Finally, it is shown that the greatly improved amorphous‐phase stability of the 2 nm Sb thin film enables robust and reversible optical switching in a silicon‐based waveguide device.
Zhang et al. (Wed,) studied this question.