My discovery process is multi-step. I typically start with my SDS100 in scan mode, scanning the particular band of interest (for example last week I was on an out-of-state road trip, and the Tier 3 system I was looking for is in the 935-939MHz range, so I searched that band). If I see a T3 signal come in, I would input it into DSD Plus on the Laptop with the SDR Radios, and see what came up. If it was the system of interest, I would continue monitoring until I ran out of range or until another frequency of interest came up on the SDS100 to replace it.
I've spent the better part of this evening parsing DSD Plus logs from the road trip (and I'm still not done) gathering the essential data to build a RRDB submission. I've also identified a number of sites that I don't have sufficient data to submit, but I will add them to the system's Wiki for others to research, or for me to go back to those areas when I visit the area again.
If it is an elusive system (for example the Beacon on Capacity+ systems), I will use the wireless survey function on DSD Plus to survey the band, looking for the tell-tale spikes on the graph, which I will then focus my attention on. That's how I identified a hospital that was using one of the 454MHz paging frequencies (not licensed to them) for one of their Capacity+ channels.