Compositions for use in tri-layer applications are described herein, wherein the composition has a matrix and includes: a formulated polymer comprising at least one type of silicon-based moiety forming the matrix of the polymer, a plurality of vinyl groups coupled to the matrix of the polymer, and a plurality of phenyl groups coupled to the matrix of the polymer, at least one condensation catalyst, and at least one solvent. Tri-layer structures are also contemplated herein that comprise an organic underlayer (first layer), antireflective compositions and/or films contemplated herein (second layer) and a photoresist material (third layer) that are coupled to one another. Methods of producing a composition for tri-layer patterning applications includes: providing a formulated polymer comprising at least one type of silicon-based moiety forming the matrix of the polymer, a plurality of vinyl groups coupled to the matrix of the polymer, and a plurality of phenyl groups coupled to the matrix of the polymer, providing at least one condensation catalyst, providing at least one solvent, providing at least one pH modifier, blending the formulated polymer and part of the at least one solvent in a reaction vessel to form a reactive mixture; and incorporating the at least one pH modifier, the at least one condensation catalyst and the remaining at least one solvent into the reactive mixture to form the composition.