Journal
VACUUM
Volume 207, Issue -, Pages -Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.vacuum.2022.111572
Keywords
Doped zinc oxide films; Thermal conductivity; Frequency domain thermoreflectance; Atom probe tomography
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This study focuses on the Bi doping effect on ZnO and the microstructure changes induced by the co-doping of Bi and Al in ZnO thin films. The results show that the introduction of Bi and Al can significantly reduce the thermal conductivity of ZnO films, with Bi mainly contributing to grain boundary scattering. However, the coexistence of Bi and Al limits further reduction in thermal conductivity due to morphological changes in the film's microstructure. The findings are important for improving thermoelectric efficiency.
The dissipation of heat generation has been one of the largest obstacles in the design of semiconductor devices and reducing the thermal conductivity is vital for improving thermoelectric efficiency. This work focuses on the Bi doping effect on ZnO, and ZnO:Al thin films produced by magnetron sputtering with thickness varying be-tween 500 and 900 nm. The approach introduces Bi ions, a higher mass element, into the ZnO metal-oxide matrix, to hinder phonon-mediated heat conduction and, consequently, reduce thermal conductivity. Atom probe tomography (APT) was employed to survey Bi doping distribution in ZnO:Al:Bi and ZnO:Bi thin films and to study the morphology of the grain boundaries. The thermal properties of the thin films were measured by frequency-domain thermoreflectance. Based on thermal conductivity results, it is concluded that the doping of ZnO films with Al has a significant effect on thermal conductivity, being reduced from 6.0 W m(-1) K-1 in its undoped state to 3.3 W m(-1) K-1 for ZnO with similar to 3 at.% of Al, mainly due to alloy scattering of phonons in the wurtzite cell. Further doping with Bi contributes to a slight reduction in the thermal conductivity of ZnO:Al.Bi films (2.9 W m(-1) K-1), due to grain boundary scattering by Bi/Bi2O3 phases. This result is understood as the confluence of two counteracting effects. On the one hand, the thermal conductivity of the film decreases because Bi, unlike Al, is segregated to grain boundaries and does not substitute Zn in the wurtzite crystal lattice, which is unequivocally demonstrated by APT results. On the other hand, the simultaneous presence of Al and Bi triggers a morphological change with the film's microstructure becoming more columnar. This change in microstructure from 3D island growth in ZnO:Al and ZnO:Bi to a more regular columnar structure in ZnO:Al,Bi limits further reduction in the thermal conductivity.
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