Wow, that was fast. I got really, really lucky. I started expanding the Riley line today and pretty quickly ran across one who married someone with a surname from one of the other genetic clusters I'm tied to (Sargent). So I followed that family and in the next generation down immediately found one who had married a Jarvis. One of their sons matches nearly all of the vague info we had gotten from my grandmother (name, locations, sibs, sib locations, etc.), plus some other corroborating info. We have FTDNA matches that link to each of his four sets of great grandparents. I'm ~99% confident that I've found my mother's father. (Now what?! More specifically, at what point can I be confident enough to actually link to him on WikiTree?)