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In this work, we have thoroughly studied the effects of flux composition andtemperature on the crystal growth of the BaCu2As2 compound. While Pb and CuAsself-flux produce the well-known {\alpha}-phase ThCr2Si2-type structure (Z=2),a new polymorphic phase of BaCu2As2 (\b{eta} phase) with a much larger clattice parameter (Z=10), which could be considered an intergrowth of theThCr2Si2- and CaBe2Ge2-type structures, has been discovered via Sn flux growth.We have characterized this structure through single-crystal X-ray diffraction,transmission electron microscopy (TEM), and scanning transmission electronmicroscopy (STEM) studies. Furthermore, we compare this new polymorphicintergrowth structure with the {\alpha}-phase BaCu2As2 (ThCr2Si2 type with Z=2)and the \b{eta}-phase BaCu2Sb2 (intergrowth of ThCr2Si2 and CaBe2Ge2 types withZ=6), both with the same space group I4/mmm. Electrical transport studiesreveal p-type carriers and magnetoresistivity up to 22% at 5 K and under amagnetic field of 7 T. Our work suggests a new route for the discovery of newpolymorphic structures through flux and temperature control during materialsynthesis.

Novel polymorphic phase of BaCu2As2: impact of flux for new phase formation in crystal growth