Raja and Sharan had a match point at 6-5 in the deciding fifth set but could not convert and ended up with a 3-6 4-6 6-4 7-6(6) 8-10 defeat against seventh seeds Raven Klaasen and Rajeev Ram in the second round.
The gruelling match lasted three hours and thirty minutes on court 6.
Rohan Bopanna's campaign also ended after he and Edouard Roger-Vasselin suffered a 6-7(6) 3-6 7-6(5) 3-6 defeat against Ken and Neal Skupski from Great Britain in a contest that lasted two hours and 28 minutes
However, Raja, Sharan, Paes and Bopanna are still in hunt in the mixed doubles event with their respective partners.
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