Crystallization and semiconductor-metal switching behavior of thin VO2 layers grown by atomic layer deposition

Crystalline vanadium dioxide (VO2) thin films were prepared by annealing amorphous VO2 films which were deposited by atomic layer deposition on a SiO2 substrate. A large influence of the oxygen partial pressure in the annealing ambient was observed by means of in-situ X-ray diffraction. In the range between 1 and 10Pa of oxygen the interesting VO2(R) phase crystallized near 450°C. Between 2 and 10Pa of oxygen, metastable VO2(B) was observed as an intermediate crystalline phase before it transformed to VO2(R). Anneals in inert gas did not show any crystallization, while oxygen partial pressures above 10Pa resulted in oxidation into the higher oxide phase V6O13. Film thickness did not have much effect on the crystallization behavior, but thinner films suffered more from agglomeration during the high-temperature crystallization on the SiO2 substrate. Nevertheless, continuous polycrystalline VO2(R) films were obtained with thicknesses down to 11nm. In the case where VO2(R) was formed, the semiconductor–metal transition was observed by three complementary techniques. This transition near 68°C was characterized by X-ray diffraction, showing the transformation of the crystal structure, by spectroscopic ellipsometry, mapping optical changes, and by sheet resistance measurements, showing resistance changes larger than 2 orders of magnitude between the low-temperature semiconducting state and the high-temperature metallic state. •Amorphous VO2 films were grown by atomic layer deposition.•Crystallization was studied by means of in-situ X-ray diffraction (XRD).•The optimal oxygen partial pressure during annealing was found to be around 1Pa.•Continuous crystalline VO2 layers down to 11nm thickness were obtained at 450°C.•XRD, ellipsometry and sheet resistance showed the semiconductor–metal transition.