Direct Evidence on Effect of Oxygen Dissolution on Thermal and Electrical Conductivity of AlN Ceramics Using Al Solid-State NMR Analysis

Aluminum nitride, with its high thermal conductivity and insulating properties, is a promising candidate as a thermal dissipation material in optoelectronics and high-power logic devices. In this work, we have shown that the thermal conductivity and electrical resistivity of AlN ceramics are primarily governed by ionic defects created by oxygen dissolved in AlN grains, which are directly probed using ²⁷Al NMR spectroscopy. We find that a 4-coordinated AlN₃O defect (O_N) in the AlN lattice is changed to intermediate AlNO₃, and further to 6-coordinated AlO₆ with decreasing oxygen concentration. As the aluminum vacancy (V_Al) defect, which is detrimental to thermal conductivity, is removed, the overall thermal conductivity is improved from 120 to 160 W/mK because of the relatively minor effect of the AlO₆ defect on thermal conductivity. With the same total oxygen content, as the AlN₃O defect concentration decreases, thermal conductivity increases. The electrical resistivity of our AlN ceramics also increases with the removal of oxygen because the major ionic carrier is V_Al. Our results show that to enhance the thermal conductivity and electrical resistivity of AlN ceramics, the dissolved oxygen in AlN grains should be removed first. This understanding of the local structure of Al-related defects enables us to design new thermal dissipation materials.