The invention provides a process to form a polymer composition comprising at least one ethylene/α-olefin/non-conjugated polyene interpolymer, and wherein the polymer composition has at least the following properties: a) a Mw/V0.1 ratio greater than, or equal to, 1.80 (g/mol)/(Pa·s); said process comprising polymerizing one or more mixture(s) comprising ethylene, an α-olefin and a non-conjugated polyene in the presence of a catalyst system comprising a metal-ligand complex of Formula (I), as described herein.