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The third seed from Romania had been looking to become the first woman to retain her title at Roland Garros since Belgian Justine Henin won three times in a row from 2005-07.
Defending champion Simona Halep's quarterfinal against Amanda Anisimova and Australian Ashleigh Barty's clash with Madison Keys will now be played on Thursday.
Naomi Osaka's quest for a third consecutive Grand Slam title almost came to an abrupt end as a number of top players struggled to book their spots in the second round of the French Open.
Arantxa was in Bengaluru as the ambassador of the upcoming TCS World 10K international marathon.
Barty became the first Australian woman since Stosur in 2013 to reach the top 10 in the world rankings.
The former world No. 1 will officially begin working with the Belgian at next week's Qatar Open.
For a place in the semifinals, Serena Williams will meet Czech seventh seed Karolina Pliskova.
The Czech seventh seed broke former Wimbledon champion Muguruza five times in the one-sided clash at Margaret Court Arena.
Top seed Halep had the odds stacked against her ahead of the Australian Open, but the Romanian proved her title credentials with a breezy 6-2, 6-3 third-round win over multiple Grand Slam winner Venus.
The 37-year-old Serena, chasing a record-extending eighth Melbourne title in the professional era, demolished Ukrainian teenager Dayana Yastremska 6-2, 6-1.