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The Serbian will now take on Russian 14th seed Nadia Petrova, who battled to overcome Safina's conqueror, unseeded Romanian Alexandra Dulgheru, winning 6-0 3-6 6-2.
CNN: Serena and Venus headed for Rome semifinal clash
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Meanwhile, up and coming Romanian Alexandra Dulgheru beat Chinese fifth seed Zheng Jie 6-3 6-4 to retain the title at the WTA event in Warsaw.
CNN: Sharapova warms up for Roland Garros with title win
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But former world number one Dinara Safina's poor form continued as she was dumped out of the competition by Romanian Alexandra Dulgheru, losing 6-4 6-7 6-1.
CNN: Venus brushes aside Schnyder in Rome
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They were joined in the second round by Francesca Schiavone (17), Alona Bondarenko (27) and Alexandra Dulgheru (31), who were all taken to three sets before triumphing.
BBC: Serena Williams and Caroline Wozniacki make progress
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Petrova will now meet Czech Lucie Safarova or Romanian Alexandra Dulgheru in the quarterfinals while Serena has had her preparations for the French Open later this month cut short.
CNN: Serena loses but Venus rises after Madrid win
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Russian seventh seed Vera Zvonareva battled past Romanian world No. 61 Alexandra Dulgheru, as last year's semifinalist won 7-6 (7-4) 6-7 (5-7) 6-3 to set up a clash with 51st-ranked Czech Lucie Hradecka.
CNN: STORY HIGHLIGHTS
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Number 14 seed Flavia Pennetta demolished her fellow Italian Roberta Vinci 6-1 6-1, 19th seed Nadia Petrova was similarly comfortable in her 6-1 6-2 win against Agnes Szavay, and Alexandra Dulgheru eased past Timea Bacsinszky 6-4 6-2.
BBC: Svetlana Kuznetsova scrapes through at French Open