I think we're probably reaching the limit for how much more we can tell you. Guiding data is only a crude tool, at best, for trying to identify mechanical problems. One point I'll make is to respond to your "instinct" that the RA guiding is simply over-shooting and probably warrants a lower aggressiveness. That's a very common mistake people make and it happens because they don't look closely at the individual guide commands. Here's an example from your data:
Look at each of the guide commands - the rectangles - and notice how many consecutive pulses it often takes to get the intended response from the mount. Reducing the aggressiveness factor will make this problem worse, not better. I will agree there are a few time periods when it does look like over-shooting but those are in the minority and there's certainly no consistency. Your problem is not with the guiding parameters, it's with the mount. You identified a time period where the RA RMS was 2x that of Dec, and it looks like this:

Where are all these big RA excursions coming from? They were completely absent in the guiding session you were happy with which, by the way, was done on the opposite side of the pier. I don't know why this is happening. Is the gear well-balanced in RA? Are these excursions originating with the actual mount tracking or from something in the payload? While this remains unresolved, I think you may need to revert to hysteresis for RA, and you probably need to reduce your guide camera exposure time in order to guide at a faster cadence. The PPEC algorithm necessarily assumes that the mount is reasonably well-behaved and that the RA tracking errors are periodic and comparatively small. Having all these wild excursions get baked into a PEC model is not what you want to happen. If you can't figure out what's going wrong, you can probably isolate whether the side-of-pier dependency is actually coming from the RA drive. By loosening the RA clutch and manually moving the scope around from one side of the pier to the other, you can effectively rotate the worm wheel by something close to 180 degrees. You have to be careful about this because the scope will no longer know where it's pointing, so a plate solve and synch will be required right away. It's just a suggestion, I wouldn't do it unless I had convinced myself that the problem isn't coming from a different source.
Sorry I can't offer any better explanations,
Bruce