Getting your FD as close as possible in the big/small setting will allow you to adjust the small/big much better. Also if you're pushing the cassette beyond 11-32t, using Ultegra 11/11t jockey wheels is highly recommended.
I found the best shift combination to be Shimano chainrings, chain and cassette. With aftermarket cassettes, I found better shift performance with KMC chains. I don't particularly like the LTwoo FD. When the new ER9/X components come out, I'll definitely look to try the new FD out (if I can buy it separately) since it has a new design.