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Intrinsic localized modes (ILMs) - also known as discrete breathers - are localized excitations that form without structural defects in discrete nonlinear lattices. For crystals in thermal equilibrium ILMs were proposed to form randomly, an idea used to interpret temperature activated signatures of ILMs in α-U and NaI. Here, however, we report neutron scattering measurements of lattice vibrations in NaI that provide evidence of an underlying organization: (i) with small temperature changes ILMs move as a unit back-and-forth between [111] and [011] orientations, and (ii) when [011] ILMs lock in at 636 K the transverse optic (TO) mode splits into three modes with symmetry-breaking dynamical structure resembling that of a superlattice, but there are no superlattice Bragg reflections and the pattern itself has crystal momentum. We conclude that this dynamical pattern is not derived from the rearrangement of atoms but from a coherent arrangement of ILMs decorating the crystal lattice in equilibrium.

Symmetry-breaking dynamical pattern and localization observed in the equilibrium vibrational spectrum of NaI