The sixth seeded Indo-Romanian duo lost 6-7 3-6 to unseeded pair of Dominic Inglot of Great Britain and Sweden's Robert Lindstedt in a contest that lasted 80 minutes on court number 17.
Inglot and Lindstedt took 44 minutes to win the first set and 36 minutes to take the second.
The Inglot-Lindstedt pair smashed five aces and 28 winners on their way to the semifinals, while Bopanna and Mergea hit six aces and 23 winners.
Bopanna is also in contention in the mixed doubles event where he and his partner Yung-Jan Chan are up against Leander Paes and Martina Hingis in the semifinals.
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