Nonlocal theory for heat transport at high frequencies

We develop a nonlocal theory for heat conduction under high-frequency temperature fields and apply the theory to explain reductions of the apparent thermal conductivity observed in recent experiments. Our nonlocal theory is an analytical solution of the Boltzmann transport equation for phonons in a semi-infinite solid, similar to a prior nonlocal theory for heat conduction under a high-temperature gradient but subjected to periodic heating at the surface. The boundary condition of periodic heating, as opposed to prior calculations of heating by a single laser pulse, better mimics time-domain thermoreflectance (TDTR) and broadband frequency-domain thermoreflectance (BB-FDTR) measurements. We find that, except for pure crystals at high frequencies, the effective thermal conductivity derived using the nonlocal theory compares well with calculations of a modified Callaway model that includes an upper limit on the phonon mean-free path at twice the thermal penetration depth. For pure crystals, however, the effective thermal conductivity derived from the out-of-phase calculations are independent of frequency, in agreement with prior TDTR measurements, due to the countereffect of reduced heat flux and diminished relative phase between the heat flux and temperature oscillations at high frequencies. Our results suggest that empirical interpretation of ballistic phonons not contributing to heat conduction is not general and can only be applied to measurements on alloys and not pure crystals, even when a large laser spot size is used in the experiments and the interfacial thermal resistance is negligible.