Four-phonon scattering is widely regarded as the leading higher-order anharmonic correction to conventional three-phonon description of anharmonic scattering and lattice thermal transport. Here, we show that diagrammatic perturbation theory contains another phonon linewidth contribution of the same perturbation order, arising from the coupling between cubic and quintic anharmonic vertices. We derive and implement this contribution from first principles and identify it as a quintic-anharmonicity-assisted three-phonon scattering channel. Although this process shares the energy-conservation structure of the conventional three-phonon process, its perturbative order and temperature dependence resemble those of the conventional four-phonon process. For Si, we find that phonon scattering from this additional channel is comparable to four-phonon scattering over a broad frequency and temperature range, leading to a similar accelerated reduction of lattice thermal conductivity at high temperatures. We further show that in strongly anharmonic AgCl, this channel can become comparable to the ordinary three-phonon scattering even at room temperature. These results demonstrate that the commonly observed high-temperature enhanced scattering and suppression of lattice thermal conductivity might not be attributed uniquely to the four-phonon process, and establish quintic-anharmonicity-assisted three-phonon scattering as a previously overlooked same-order channel in anharmonic lattice dynamics, which may be leveraged to uncover hidden microscopic thermal transport mechanisms.

Close

PrevNext

View figure in article

• Anharmonic lattice dynamics
• Phonons
• Thermal conductivity