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PoetryNEmotion I appreciate your question more than you know. I would not know where to start with him. I was a young teen bound for the military draft when his/and CSN broke in with their music. Many had come out of former cool bands like Buffalo Springfield, the Hollies....where they picked up Graham Nash's superior high vocal notes, the Byrd's bandsman (and recently deceased) David Crosby.....
Hah, if you knew me, you would never ask the question because quite simply, I am totally incapable of choosing one piece. I could point to his split with the band and his sojourn with Manassas, his solo pieces such as Tree Top Flyer which is over the top cool acoustic.....I mean, for me, from the days of my youth to this day Steven IS a friggin' icon. I've no other way to describe him.
Pick through his stuff if you're into it. He is so gifted and unique. The only thing, if at all, I could add in a "favorite" type thing is that, he is my favorite musician....and that is saying a host of things my friend.
Get into him, and dig on the early to late stuff. I never want this dude to pass....
That's where I'm at with the man. I've seen him live.....such good stuff. Straight up.