Phononic Frequency Combs in Twisted Bilayer Transition Metal Dichalcogenide Heterostructures from First Principles

Abstract

Phononic frequency combs are equidistant spectral ladders generated when a driven vibrational mode transfers energy to an autoparametrically excited subharmonic mode through anharmonic intermode coupling. In previous studies, the coupling strength governing this energy transfer has typically been treated as a free parameter, extracted from a fabricated device, or adopted from an earlier calculation for a specific mode pair. As a result, whether a given crystal can support a phononic frequency comb, and the drive strength required to generate it, has not been predictable a priori. Here we obtain the complete parameter set from density functional theory. Twisted bilayers of \MoSSe{} and \MoSMoSe{} at the commensurate angle $21.787^{\circ}$ adopt space group $P3$ in a 42-atom \rootseven{} moiré supercell. The second-order force constants provide the mode frequencies; the third-order constants provide the linewidths through the Boltzmann transport equation and hence the quality factors; and the same third-order tensor projected onto the phonon eigenvectors of a chosen mode pair provides the anharmonic couplings $\kt$ and $\kss$. Both bilayers constitute a mode pair within $0.8\%$ of the $2\!:\!1$ resonance with $ω_1/ω_2 = 1.9923$ in \MoSSe{} and $1.9943$ in \MoSMoSe{}. By integrating the resulting two-mode equations, both modes generate combs through a discontinuous transition: at $701\,\fth$ in \MoSSe{} the envelope variance rises from $2.1\times10^{3}$ to $1.37\times10^{4}$ and the tooth count of mode 1 from 7 to 16 within a single $5\,\fth$ increment, identifying the onset as subcritical. The spectral entropy peaks \emph{before} this jump, at $341\,\fth$. The two compounds carry comparable coupling, differing by a factor of $1.2$. However, the comb excitation threshold is set by the quality-factors of signal modes: $Q_2 = 672$ for \MoSSe{} and $Q_2 = 3844$ for \MoSMoSe{}.