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Damping of phonon momentum suppresses the lattice thermal conductivity (kl)through low energy acoustic-optical phonon interactions. We studied the thermaltransport properties and underlying mechanism of phonon interactions in thelarge unit cell Cu26V2Sn6Se32. The large number of atoms in the unit cellresults in low acoustic phonon cutoff frequency, flat phonon branches, lowfrequency Raman active modes, localized rattler-like vibrations and strongcrystalline anharmonicity. The crystal structure complexity disrupts the phononpropagation through weak bonded Cu atoms, boson peak and poor phonon velocity.The sulfur at selenium sites (Cu26V2Sn6Se30S2) distort the crystal lattice byoffering additional scattering mechanism at the anionic sites, therebyincreases the power factor and decreases the kl. This strategic manipulation ofphonon scattering towards ultra-low kl not only results in improvedthermoelectric performance but also offers insights into the fundamentalunderstanding of heat transport in complex structured, large unit cellcompounds.

Ultralow Lattice Thermal Conductivity in Complex Structure Cu26V2Sn6Se32 due to Interaction of Low-Frequency Acoustic-Optical Phonons