Yes, the 3.6 and tubes are not the best match. The 3.6 like beefy solid state amplification.
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The Theil websites says they need 100-500wpc. Your Primaluna is 70-96 wpc depending on configuration.
So, you are really at the bottom of the spectrum. Adding in the 2 ohm minimum of the Theil's and you are taxing the amp.
You could try a pair of Zero Autoformers to help with the low impedance, but a higher rated amp is probably the best way to go.
Those Theil's were one of the last of Jim's designs, so I would probably keep them. If you did want to change, I would recommend Vandersteen-both use time and phase alignment, and results in a similar sound reproduction.
For amps, you could get an old McCormack DNA-1 and have Steve upgrade it. (Buy a non working unit and save more. Steve guts the amp and installs a new board, so it doesn't need to be working). For Tube amps I would recommend Atma-Sphere.
Here is one review with Theil speakers;
I own the Thiel CS 3.6 speakers and you don't want to drive them with minimal power, because they won't sing. Plus, you'll get distortion if you push it. I first went the tube route, and today would go with a quality SS amp and perhaps an equally good tube preamp. I'm in the hunt myself for a proper amp for my Thiels for a system to be set up in my basement family room. Either way you go, your amp and your speakers must be optimized for one-another. A lesson that took me too long to get right.
I see now you sold the Thiels and kept the PL amp, this amp has a peaking high frequency that starts at 10k, only a 2ohm load flattens it out (green trace) a speaker that seems subdued in this area or one that has a 2ohm load in this area will be a good match to look for.
Maybe look at Martin Logans ESL’s that have active (200w) bass like the Montis, because ML’s do have a 2ohm load in the HF this will nullify the PL’s peak and the ML having an active bass means the PL won’t have to do it which will be it’s weak area. The more I think of it, this could be a match made in heaven, but not for party levels as you have limited wattage from the PL.