I can only assume that the 4:30am arrival time is dictated by the slot requirements. Otherwise there

Access to Sao Paulo for US Airways was part of the deal they struck to trade slots with Delta at LaGuardia and Washington s National airport. Now US Airways has finally houston luxury hotels announced their intended schedule of service for the route . Starting on May 5, 2013 the carrier will offer daily service on their 767-200 aircraft.
The 4:30am arrival in Sao Paulo is just over an hour before the bus service into town starts up. Most days they ll be vying with the TAM inbound from Madrid to see which is the first international arrival of the morning. That could be good in the form of shorter immigration and customs lines or it could be a mess with limited service available. The plane sits on the ground for a few hours at that point before turning around back to North America that same day. Most carriers fly both to and from Brazil as an overnight flight; US Airways is choosing houston luxury hotels to not leave a plane on the ground all day to make that happen. American Airlines and TAM both also have daytime flights but those two carriers offer both daytime and the overnight options (and more destinations at both ends).
And the 8:25am departure on the north-bound flight is mighty early. With the traffic in general and the distance from GRU to town that means a 5:30ish departure from the hotel in the morning to get going. Maybe 6am if you re feeling a bit aggressive.
I can only assume that the 4:30am arrival time is dictated by the slot requirements. Otherwise there is nothing stopping the carrier from leaving an hour later and having a more reasonable arrival time in Brazil and better inbound connections in Charlotte. At least for the return it would seem that they need the aircraft to continue on to Europe at some point that same night, necessitating the earlier departure.
Given the times in Charlotte, they re using different aircraft in each direction. Maybe the arrival times argument will be mitigated somewhat by the positioning houston luxury hotels flight having lousy on-time performance.
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