NIST BSCCO Phase Equilibria

Primary Phase Fields

By definition, a primary phase is the first crystalline phase to appear on cooling a composition from the liquid state. A primary phase field is the locus of all compositions in a phase diagram having a common primary phase. The primary phase field of a binary phase is a curve, that of a ternary phase is a surface, and that of a quaternary phase can be described as a volume. Therefore, in the 4-component Pb-free BSCCO system, the primary phase field of the 2212 phase is represented by a volume, and for the (Bi,Pb)-2223 phase, the primary phase field is a multidimensional volume.

In order to obtain the primary phase field of a given phase of interest, the first step is to determine all compounds that are in equilibrium with the phase of interest. Next, the multiphase compatibility regions involving this phase are identified. For example, in a ternary system, one would determine all 3-phase compatibility regions involving the ternary phase of interest, or 4-phase compatibility regions in a quaternary system, or five-phase volumes in a five-component system, etc. For each of the compatibility regions, the onset melting temperature is then determined. The set of compositions of the first liquids formed in each of these regions will determine the outline of the primary phase field.

The compositions of the multi-phase volumes were modeled using a computational geometry technique based on forming a convex hull from the experimentally determined chemical compositions.  This mathematical notion of a the convex hull, the smallest convex set of points that contains all of the given data points, has been used in many physical science applications. In this case, the convex hull represents the extent of the compositional volume. This numerical procedure results in a well-formed, hyper-volume in 5-dimensional space. It is important to note the requirement that chemical compositions sum to unity results in the loss of one degree of freedom.  In general the convex hull is defined by the matrix equation Ax + b < = 0 where A is a matrix whose rows define the unit normal vectors to the faces of the convex hull. Each element of the vector b defines the proximity of the given face to the origin of the multi-dimensional space. The vector x gives the coordinates corresponding to a given point. The matrix A and vector b can be found using a so-called "sweeping algorithm''. When the procedure is complete, the matrix A has dimension k × 5 and the vector b has dimension k where k is the number of faces in the convex hull.
 
This equation can be used to determine if a given composition lies inside the (Bi,Pb)-2223 primary phase field. If Ax-b <  0, the particular composition lies inside the crystallization volume. If the value of all components is zero, the composition is on the surface; and if the value of any one component is positive, it is outside the volume. Compositions falling outside this volume should be avoided for the processing of the 2223 phase, as they would be expected to produce large primary crystals of unwanted phases.