So you have made a major change in your keywords?
It will probably take several days to weeks for Google to recognize the change.
You DO need to do off-site optimization using your new keywords! Write lots of articles, using your new keywords in your text links in your authors sig box.
Also, try to get back links from related sites - using your new keywords as anchor text, of course.
When you go in and completely makeover your sites keywords, it will take some time to get it geared towards those keywords. Just keep working, and do what you did with your old keywords if that worked well!
I hope this is what you're asking.