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I'd really appreciate any input on how to establish this effect without the large file size. Manual modifications, different programs, different formats, anything that works!
"Optimizing" them within the program means reducing the # of colors
This is what optimizing is. The problem you ae probably experiencing is that you have no control over the degree of optimization. You might possibly look around in any options settings that might give you control, or look closely at any in-between dialogues that specify color depth/colors in palette.
IMO animation is a bad idea from the outset, for all the reasons you will find on Google and this site. But if you think this is the way to go, your best option is to use Flash. You will have adequate control over your animation image quality and additionally it will stream, loading content as it's required. Granted, this is a big leap from animated .gifs and presents it's own set of difficulties, but if I had to do animated banners I'd do it with Flash.
I seem to recall that you can save a background for the animation, if appropriate, and then reduce the frame images by removing the background. Might save a bit there.
I haven't tried this for a few years so I'm afraid I can't remember how it is done or if it will save much, but a good editor should have a destruction, I mean instruction manual.
I used JASC Animation Shop I think.