“…The choice of PEO as the model system presents an opportunity to benefit from the extensive fundamental studies of its crystallization behavior, 23,24 rheological response 25−28 (including by the coauthors 29−33 ), and fiber formation using electrospinning (ES) and centrifugal force spinning (CFS), as discussed herein. Despite the relative success of ES for producing submicron and nanoscopic fibers using various polymers, the need for high voltage sources, low production rates, and limited range of spinnable formulations has driven the search for alternatives [4][5][6][7]10,34,35 including CFS, 6,35−37 melt-blown, 38,39 template synthesis, 40 phase separation, 41 and CO 2 laser supersonic drawing, 42 among others. However, designing applicationready fibers involves multifaceted challenges 1−6,21,28,34−56 related to correlating the processing parameters and formulation properties, including rheological response to the trinity of spinnability, morphology, and properties that we refer to as the fiber engineering trifecta.…”