Photoluminescence Detection of Polytype Polarization in r-MoS2 Enabled by Asymmetric Dielectric Environments

Abstract

The rhombohedral (r) polytypes of transition metal dichalcogenides (TMDs) constitute a novel class of two-dimensional ferroelectric materials, where lateral shifts between parallel layers induce reversible out-of-plane polarization. This emerging field, known as SlideTronics, holds significant potential for next-generation electronic and optoelectronic applications. While extensive studies have investigated the effects of electrical and chemical doping on excitonic signatures in 2H-TMDs, as well as the influence of dielectric environments on their optical properties, the impact of intrinsic polarization in asymmetric environments remains largely unexplored. Here, we demonstrate a striking polarization-dependent photoluminescence (PL) contrast of up to 400\% between ferroelectric domains in bilayer and trilayer rhombohedral molybdenum disulfide (r-MoS2). This pronounced contrast arises from an asymmetric dielectric environment, which induces polarization-dependent shifts in the Fermi energy, leading to a modulation of the exciton-trion population balance. A detailed temperature-dependent line shape analysis of the PL, conducted from 4K to room temperature, reveals domain-specific trends that further reinforce the connection between polarization states and excitonic properties. The persistence of these distinct optical signatures at room temperature establishes PL as a robust and non-invasive probe for ferroelectric domain characterization, particularly in fully encapsulated device architectures where conventional techniques, such as Kelvin probe force microscopy, become impractical.