Prompted by your post, I've just spent a few days experimenting with different Pi versions. My system is rpi/allo signature -> rme adi-2 dac > active nytech/arc amp & speakers.
Software is picoreplayer 6.1.0 on the player and LMS server, either 7.9.2 on a VM, or 8.0.0 on the same Pi. music is stored on a NAS.
I started with a PI3(1Gb), then swapped to a Pi4(4Gb) that I happened to have already. and then to a new Pi4(8Gb)
And I heard an astonishing improvement just going from the Pi3 to Pi4/4Gb - much as you described - more real vocals, cleaner bass, just more enjoyable.
BUT - that change was going from Pi3 to Pi4. I did not hear any convincing difference going from Pi4 4Gb to 8Gb, nor from moving the LMS server to the Pi, nor from going from LMS 7.9.2 to LMS 8
I'm sure that the 4Gb to 8Gb should have NO impact. And that's what I (didn't) hear. Today my Pi4 is only using 1.5Gb of ram. Having 2.5Gb or 6.5Gb unused cannot make a difference. (I'm a software guy - I KNOW this.) Is it possible that the Pi4/8GB, being a later version, has had other changes, apart from ram, from the 4Gb model?
But I have no idea why going from Pi3 to Pi4 should make a difference either (but it did for me). But this was a much bigger change in h/w - faster cpu, 1G -> 4G ram, better usb and network h/w, so at least an improvement here is possible. (and the fact that my Pi4 today is using 1.5Gb ram implies that the 1Gb Pi3 was at least partly constrained by ram (but not the Pi4/4Gb)
And moving LMS from a separate machine to the Pi4 made no audible difference, but it's more convenient there, so I'll leave it as is.
So more questions than answers - sorry.
A thought - you heard a difference moving to an 8Gb Pi4 from a 2GB one, which subsequently 'blew up'. Could the 2GB pi have been faulty in some way, and havecontributed to the differences you heard?
But bottom line. my PI-based streamer sounds better today than last week, after changes prompted by your post, so thank you.
khozmo passive pre/nytech ca252/cxa252 amps, arc 101 speakers
vinyl: --- lp12/kore/lingo4/ekos2/dv 10x5/gs accession
digital: --- caiman SEG/allo digione, synology nas, rotel 965 cd