I'm very much surprised noboby else has replied.
As planned, I started playing all five score albums this morning; Season 2 is about to end now.
My opinion of it is much better; somehow I had the vague impression that this an Season 3 had much more suspense / creepy music, that overweighed the simple, lyrical, beautiful material; I was wrong (though I still have to go through the third album).
There is much to love in here.
Reading the scene synopses for each track on Lostpedia helps a lot; this is the kind of score that needs contextualizing for a good many tracks so that you may remember what it's about and appreciate the music even more by understanding why it's doing such and such thing.
I probably had not been able to play those seasons in the best conditions, whether the first time or the following chances I gave them; this time, I can pay full attention, and (silly as it may seem, obvious as it is), I find the album is not so different from the first one.
It's a great (re)discovery. It's is easier for me to point out the thematic tracks, and Season 2 has a very nice share of those: "Mess It All up", "Hurley's Handouts", "The Gathering", "Shannon's Funeral", "All's Forgiven... Except Charlie", "The Last to Know", "Rose and Bernard".
The easy way out is to advise you to get all the albums, Roger.
To answer your request, I can narrow it down to Seasons 1 and 4.
If you really insist on having only one recommendation, I would be tempted to say Season 4, but it would be a shame not to have such wonderful tracks as the final two from Season 1, so I'm really hard pressed to choose between those two albums.
Update: Season 3 is like Season 2; I'm rediscovering it and cursing the Others for preventing me from doing so before.
However (very) good it is, I believe having the whole of the score for the season's finale may have also affected my opinion, as it is made up of many small bits and pieces; the selections from various episodes on the other CDs help make for a better listening experience-- though, again, what I hear now pleases me more than I remembered. A little pruning down might have helped.
Second Update: Season 4 playing; this definitely is the strongest album, along with the first one, with the added advantage of lots of material to work with and develop, a lot of action and strong emotional moments (Desmond's mind trips through time, "Ji Yeon", the finale, ...).
Enjoy the Finale!
(I'll watch it tomorrow evening)
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