Modulation of Polarization and Metallicity in Janus Sliding Ferroelectrics

TL;DR

This study uses density functional theory to explore how intrinsic electric fields in Janus sliding ferroelectric TMD bilayers can be used to modulate polarization and electronic properties, revealing pathways to design low bandgap ferroelectrics and ferroelectric metals.

Contribution

It demonstrates the tunability of polarization and bandgap in Janus TMD sliding ferroelectrics through intrinsic electric fields and stacking configurations, introducing new design principles.

Findings

Intrinsic electric fields modulate polarization and band structure.

Stacking configurations influence interlayer distance and properties.

Janus trilayers show enhanced polarization and bandgap reduction.

Abstract

Sliding ferroelectricity is emerging as a distinct and promising mechanism for realizing ferroelectricity in low-dimensional systems, offering new design principles beyond the conventional ferroelectric mechanism. Further, the coexistence of the out-of-plane polarization with in-plane conductivity induced by electrostatic charge doping makes these systems strong candidates for realizing ferroelectric metals. Using density functional theory calculations, we analyze the transition metal dichalcogenides (TMDs) based Janus sliding ferroelectric bilayers XMY (M = Mo, W; X, Y = S, Se, Te; X $\neq$ Y). In addition to exhibiting switchable interlayer polarization, Janus sliding ferroelectrics possess an intrinsic electric field within each monolayer, arising from the electronegativity difference between the chalcogen atoms. We discover that the intrinsic electric field of the monolayers can be used to modulate the interlayer ferroelectric polarization and the electronic band structure. We identify the decrease in the interlayer distance due to a particular stacking of the Janus bilayers as a major contributor to increasing polarization and reducing the bandgap. The direction of the intrinsic electric field within the Janus monolayers plays a significant role in the modulation of layer-wise contribution in the valence and conduction bands, which influences the polarization reduction due to extrinsic charge dopants. Extending this concept to Janus trilayers, we observe further enhancement in polarization and additional bandgap reduction compared to their bilayer counterparts. These results highlight the tunability of TMD-based Janus sliding ferroelectrics and suggest a pathway for designing low bandgap ferroelectrics and potential ferroelectric metals.