Two-dimensional materials (2DMs) that are stacked vertically with a certain twist angle provide new degrees of freedom for designing novel physical properties. Twist-related properties of homogeneous bilayer and heterogeneous bilayer 2DMs, such as excitons and phonons, have been described in many pioneering works. However, twist-related properties of homogeneous trilayer 2DMs have been rarely reported. In this work, trilayer MoS with the twisted angle of 12° by optimized vapor deposition rather than the conventional mechanical stacking method was successfully fabricated. The inversion symmetry of trilayer MoS is changed by twist. Phonons and excitons produced by twist have an enormous influence on the interlayer interaction of trilayer MoS, making trilayer MoS appear to have exotic optical properties. Compared with monolayer MoS, the phonon vibration and photoluminescence intensity of trilayer MoS with one-interlayer-twisted are significantly improved, and the second harmonic generation response in the non-twist region of trilayer MoS is ∼3 times that of monolayer MoS. In addition, interlayer coupling, inversion symmetry, and exciton behavior of the twist region show regional differences. This work provides a new way for designing twist and exploring the influence of twist on the structures of 2DMs with few layers.
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