So, when would be the best time to hold a unification referendum from a republican perspective? Wait until there’s a clear majority to avoid what happened when Scottish nationalists held their independence referendum in 2016? Or sooner to take advantage of the widespread dissatisfaction with Brexit in Northern Ireland?
Other than this poll (and, for this reason, I find the result somewhat suspect), there is a lot of evidence that Catholics in Northern Ireland, especially younger Catholics, are becoming progressively less nationalist, so that even though demographic trends in Northern Ireland clearly point (for now) to a Catholic majority in the long term, it may not be a nationalist majority. Brexit might be changing those minds in the short term, at least.
On the other hand, the continued economic success of Ireland and struggles of the UK (and, even more so, of Northern Ireland in particular) may put a different twist on the issue in the future.
Have you seen election results from before the 1980s? They are worth looking at and they get at your questions. They were really weak for Catholic parties, way below what numbers would suggest. Suggestive instead that Catholic attitudes to republicanism and nationalism in NI are largely a function of medium-term organisation and passion within the community, rather than long-term changes in opinion.