Oxo-hydroxo Group 5 metal clusters are an untapped resource to study and advance aqueous solution processing of metal oxide thin films. The tetramethylammonium (TMA) hexatantalate salt (TMA6[H2Ta6O19]) yields dense Ta2O5 films (~95% of the bulk ß-Ta2O5 density) with atomically smooth surfaces (<4 Å root mean square surface roughness). This same...