Within the Atlanta city limits, you need to look at Candler Park, Lake Claire, Inman Park, Virginia Highland, Morningside, Poncey Highland, or Midtown. The first three are districted to Lin Elementary, the latter four neighborhoods are districted to Morningside Elementary. Both of these are top notch elementary schools. Morningside and Lin feed into Inman Middle and Grady High. The middle and high schools are also excellent.
You can check these schools out at the GA Dept of Education website. Here is the link....
The Governor's Office of Student Achievement
Greatschools.net also has a lot of info on Atlanta schools.
Grant Park has a charter school called the "Neighborhood Charter School." It is part of the Atlanta system. I have a friend or two with kids there and I have heard that it is very good. You can find out info on it at the GA DOE website. I have even heard that there is a new charter school in East Atlanta Village, but I don't know much about it. I don't know if these charters feed into Inman Middle or Coan Middle so you would have to check into that. Coan is not a very good middle school.
You could also check out Toomer Elementary in Kirkwood. Toomer has historically struggled, but a group of parents with young children have been working very hard to improve achievement at that school. There is a parent coalition that you would have to get in touch with on that. I would imagine that if you find a realtor that knows that area well, they could get you in touch with someone involved with the coalition.
What is your price range for a home?