Direct observation of ferroelectricity in two-dimensional MoS2

Abstract Recent theoretical predictions of ferroelectricity in two-dimensional (2D) van der Waals materials reveal exciting possibilities for their use in scalable low-power electronic devices with polarization-dependent functionalities. These prospects have been further invigorated by the experimental evidence of the polarization response in some transition metal chalcogenides (TMCs)—a group of narrow-band semiconductors and semimetals with a wealth of application potential. Among the TMCs, molybdenum disulfide (MoS₂) is known as one of the most promising and robust 2D electronic materials. However, in spite of theoretical predictions, no ferroelectricity has been experimentally detected in MoS₂, while the emergence of this property could enhance its potential for electronics applications. Here, we report the experimental observation of a stable room-temperature out-of-plane polarization ordering in 2D MoS₂ layers, where polarization switching is realized by mechanical pressure induced by a tip of a scanning probe microscope. Using this approach, we create the bi-domain polarization states, which exhibit different piezoelectric activity, second harmonic generation, surface potential, and conductivity. Ferroelectric MoS₂ belongs to the distorted trigonal structural 1T” phase, where a spontaneous polarization is inferred by its P3m1 space-group symmetry and corroborated by theoretical modeling. Experiments on the flipped flakes reveal that the 1T”-MoS₂ samples consist of the monolayers with randomly alternating polarization orientation, which form stable but switchable “antipolar” head-to-head or tail-to-tail dipole configurations. Mechanically written domains are remarkably stable facilitating the application of 1T”-MoS₂ in flexible memory and electromechanical devices.