Broadband phonon-velocity suppression and a finite anisotropic crossover in twisted bilayer SnSe

Moiré superlattices reshape lattice dynamics without altering chemical composition, yet how crystal anisotropy modifies this control remains unclear. We combine density-functional-theory (DFT)-calibrated lattice-dynamical calculations with angle-matched untwisted controls to study puckered bilayer SnSe across seven commensurate twist angles (${3.18}^{\circ }$–${8.77}^{\circ }$). At 300 K, twisting suppresses the band-path heat-capacity-weighted mean-square group velocity to 2.6–8.4% of the control values; the suppression spans a broad frequency range rather than a few soft branches. The velocity response crosses over between ${4.78}^{\circ }$ and ${3.82}^{\circ }$ into a regime where the relaxed stacking textures and frequency-resolved velocity profiles become self-similar, with the normalized mean-square velocity ratio spanning only 11.1% of its mean across the three smallest angles—a finite anisotropic crossover, not a singular-angle condition. Direct DFT–MACE force-constant agreement ($r=0.996$), uniform $4\times 4\times 1$ stability scans, and acoustic-sum-rule and path-density tests support the trend. The equilibrium trend is defined by six structures after excluding one relaxation-sensitive case. These results extend phonon twistronics to low-symmetry layered materials and identify crystal anisotropy as a key determinant of finite-angle phonon crossover behavior.