Simultaneous determination of the phase boundary thermal resistance and thermal conductivity in phase-separated TiO2 thin films

Phase boundaries, most often between crystalline and amorphous phases of a material, are ubiquitous lattice imperfections in thin films, particularly deposited by low temperature processes such as atomic layer deposition (ALD). Thermal resistances from these boundaries may impede phonon transport and reduce thermal conductivity. However, to date, there have been no reports on the direct measurement of the phase boundary thermal resistance, due in part to challenges associated with fabricating an atomically flat yet geometrically planar interface between different phases within a film. Here, we present a systematic study to simultaneously determine the phase boundary thermal resistance and thermal conductivity in a series of phase-separated titanium oxide (TiO ₂ ) thin films prepared via plasma-enhanced ALD (PEALD). A precise implementation of per-cycle plasma treatment enables extremely localized crystallization—i.e., plasma-assisted atomic layer annealing (ALA)—and the fabrication of crystalline/amorphous layered structures with their respective thicknesses systematically varied. Frequency-domain thermoreflectance measures the effective thermal conductivity of each film and its top and bottom interfaces, confirmed independently using time-domain thermoreflectance. We simultaneously solve a system of linear equations generated by applying a series resistor model to each film, yielding the phase boundary thermal resistance of 5.1 m ² K GW ^–1 between crystalline and amorphous TiO ₂, as well as the thermal conductivities of 5.1 and 2.1 W m ^–1 K ^–1 for crystalline and amorphous TiO ₂, respectively. The results suggest that the crystalline/amorphous phase boundary acts like a layer of crystalline (amorphous) TiO ₂ with equivalent thickness ∼26 (∼11) nm.