Just got an email from FreshDirect - they're plugging in the people left out between Carroll Gardens and Park Slope. The new coverage is bounded by Fulton St and Flatbush to the north, joins into the existing coverage to the west at Smith St and the east at 4th Ave, and continues down to the BQE in the South. They commence deliveries to this area on 1 Dec.
(although I have to admit, I've yet to use FD. A Wegmans opened up near my office in NJ, which has some great produce with pretty decent prices...)