Impact of Relative Humidity during Spin-Deposition of Metal Oxide Thin Films from Aqueous Solution Precursors

Relative humidity during the spin-processing of thin film solution precursors is often not controlled or measured, and its effect on film thickness is generally unappreciated. Herein, we report that the relative humidity during spin-processing has a marked impact on the film thickness of amorphous metal oxide (aluminum oxide and lanthanum zirconium oxide) and hafnium oxide-sulfate (HafSOx) thin films deposited from aqueous precursors. In the humidity range studied [20–95% relative humidity (RH)], film thicknesses varied by a factor of nearly 3, and this effect is independent of the metal precursor identity. Our data suggest that film thickness depends linearly on evaporation rate (100 – RH) for all systems studied, suggesting this effect is predominantly due to the unique characteristics of water as a solvent. In situ X-ray reflectivity studies of HafSOx films deposited under different humidities reveal that, while the thickness varies significantly with humidity, the density of the as-deposited films is similar, suggesting that humidity primarily affects the relative amount of material deposited. Because reproducible film thickness is critical for many applications, our data highlight the importance of controlling humidity during spin-processing.