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A solid with larger sound speeds exhibits higher lattice thermal conductivity(k_{lat}). Diamond is a prominent instance where its mean sound speed is 14400m s-1 and k_{lat} is 2300 W m-1 K-1. Here, we report an extreme exception thatCuP2 has quite large mean sound speeds of 4155 m s-1, comparable to GaAs, butthe single crystals show a very low lattice thermal conductivity of about 4 Wm-1 K-1 at room temperature, one order of magnitude smaller than GaAs. Tounderstand such a puzzling thermal transport behavior, we have thoroughlyinvestigated the atomic structure and lattice dynamics by combining neutronscattering techniques with first-principles simulations. Cu atoms form dimerssandwiched in between the layered P atomic networks and the dimers vibrate as arattling mode with frequency around 11 meV. This mode is manifested to beremarkably anharmonic and strongly scatters acoustic phonons to achieve the lowk_{lat}. Such a dimer rattling behavior in layered structures might offer anunprecedented strategy for suppressing thermal conduction without involvingatomic disorder.

Dimer rattling mode induced low thermal conductivity in an excellent acoustic conductor