Interlayer Coupling Dependent Discrete H → T′ Phase Transition in Lithium Intercalated Bilayer Molybdenum Disulfide

In this work, the interlayer coupling dependent lithium intercalation induced phase transition in bilayer MoS2 (BL-MoS2) was investigated using an atomic-resolution annual dark-field scanning transmission electron microscope (ADF-STEM). It was revealed that the lithiation induced H -> T' phase transition in BL-MoS2 strongly depended on the interlayer twist angle; i.e., the H -> T' phase transition occurred in well-stacked H phase BL-MoS2 (with a twist angle of theta(t) = 0 degrees) but not for theta(t) not equal 0 degrees BL-MoS2. The lithiated BL-MoS2 appeared in homophase stacking, either T'/T' or H/H (locally, no phase transformation) stacking, without any heterophase stacking such as H/T' or T'/H observed. This finding indicated the H -> T' phase transition occurred via a domain-by-domain mode rather than layer-by-layer. Up to 15 types of stacking orders were experimentally identified locally in lithiated bilayer T'-MoS2, and the formation mechanism was attributed to the discrete interlayer translation with a unit step of (m/6a, n/6b) (m, n = 0, 1, 2, 3), where a and b were the primitive lattice vectors of T'-MoS2. Our experimental results were further corroborated by ab initio density functional theory (DFT) calculations, where the occurrence of different stacking orders can be quantitatively correlated with the variation of intercalated lithium contents into the BL-MoS2. The present study aids in the understanding of the phase transition mechanisms in atomically thin 2D transition metal dichalcogenides (TMDCs) and will also shed light on the precisely controlled phase engineering of 2D materials for memory applications.

Automated summary

This study used experimental and theoretical methods to investigate the lithium intercalation induced phase transition in bilayer MoS2, revealing a correlation between the phase transition mode and stacking orders. The findings contribute to the understanding of phase transition mechanisms in 2D materials and advance the precise control of phase engineering in 2D materials for memory applications.