Phonons in twisted transition-metal dichalcogenide bilayers: Ultrasoft phasons and a transition from a superlubric to a pinned phase

Abstract

The tunability of the interlayer coupling by twisting one layer with respect to another layer of two-dimensional materials provides a unique way to manipulate the phonons and related properties. We refer to this engineering of phononic properties as "Twistnonics". We study the effects of twisting on low-frequency shear (SM) and layer breathing (LBM) modes in transition metal dichalcogenide (TMD) bilayer using atomistic classical simulations. We show that these low-frequency modes are extremely sensitive to twist and can be used to infer the twist angle. We find unique "ultra-soft" phason modes (frequency $\lesssim 1\ \mathrm{cm^{-1}}$, comparable to acoustic modes) for any non-zero twist, corresponding to an \textit{effective} translation of the moir{\'e} lattice by relative displacement of the constituent layers in a non-trivial way. Unlike the acoustic modes, the velocity of the phason modes is quite sensitive to twist angle. As twist angle decreases, ($\theta \lesssim 3^{\circ},\ \gtrsim 57^{\circ}$) the ultra-soft modes represent the acoustic modes of the "emergent" soft moir{\'e} scale lattice. Also, new high-frequency SMs appear, identical to those in stable bilayer TMD ($\theta = 0\degree/60\degree$), due to the overwhelming growth of stable stacking regions in relaxed twisted structures. Furthermore, we find remarkably different structural relaxation as $\theta \to 0^{\circ}$, $\to 60^{\circ}$ due to sub-lattice symmetry breaking. Our study reveals the possibility of an intriguing $\theta$ dependent superlubric to pinning behavior and of the existence of ultra-soft modes in \textit{all} two-dimensional (2D) materials.