Heterogeneous nucleation of YBCO via fluorine based MOD process: thermodynamic and kinetic approach

Abstract The nucleation of YBa 2 Cu 3 O 7−δ (YBCO) film deposited via metal organic decomposition (MOD) approach is a complex process that has a key role in YBCO film crystalline orientation and, consequently, superconducting properties. Up to now, several studies have been carried out to clarify this step in the fluorine based MOD route which employs only or partially metals trifluoroacetate for the precursor solution preparation. However, these previous works provided only qualitative indications, whereas a quantitative theoretical investigation seems to be still lacking. In this paper, the free energy for critical nucleus formation of fluorine based MOD YBCO has been determined according to the classical nucleation theory. The volume contribution to the free energy is computed using thermodynamic data on (Y, Ba, Cu, O) systems available from the literature. The free energy barrier for nucleation depends upon nucleus orientation, via the work of adhesion and surface energies of vacuum/nucleus interfaces. The model is applied to describe heterogeneous nucleation of YBCO on (001) SrTiO 3 single crystal and provides quantitative information on nucleation barriers as a function of temperature and both precursor and gas phase compositions. Through a kinetic approach, the energy barriers are further employed to estimate the fraction of c -oriented nuclei as a function of temperature and water partial pressure. Comparison with experimental data from literature lends support to the proposed computations. Therefore, the results shown in this work may be useful in designing the YBCO deposition process in order to obtain films with superior superconducting properties avoiding expensive and time-consuming experimental optimizations.