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She made her Grand Slam debut at the French Open in 2005 and made it to the second round, where she lost to Amélie Mauresmo. In 2006, she reached the second round again by beating Virginia Ruano Pascual of Spain in the first round. She could not repeat this performance in 2007, as she lost in the first round to Venus Williams 6–4, 6–3. Cornet was defeated in the Wimbledon 2007 qualifying event by Olga Govortsova 7–6(12), 3–6, 6–4, but made it to the main draw as a lucky loser when Li Na of China withdrew. Alizé reached the second round before being defeated by the experienced Ai Sugiyama 6-0, 6–0. Also in 2007, she won a $50000 ITF tournament in Dnipropetrovsk, beating Stefanie Vogele 6–4, 6–3 in the final. In the 2007 US Open, Cornet lost to Jelena Janković in the 3rd round 4-6 6-2 6-3.
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