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It was the latest in a string of upsets that has jolted the tournament, with defending champion Roger Federer and Rafael Nadal knocked out in the first three days — along with Maria Sharapova and Victoria Azarenka on the women's side.
The International Tennis Federation said it believed the previous high total for one day at a major tournament was five, which happened on the first day of competition at Wimbledon last year, June 25.
Federer's loss ended his record streak of reaching at least the quarterfinals at 36 consecutive Grand Slam tournaments, a run that began at Wimbledon in 2004, shortly after a third-round exit at that year's French Open.
Williams is looking for her sixth Wimbledon title and improved her career record to 68-8 at the All England Club. She extended her career-best winning streak to 32 matches.
Opening the tournament on Centre Court as defending champion, Federer looked right as home as he dismantled Victor Hanescu of Romania 6-3, 6-2, 6-0 in just 68 minutes.
Darcis of Belgium stunned the two-time champion 7-6 (4), 7-6 (8), 6-4. He ended Nadal's 22-match winning streak and eliminated one of the Big Four of men's tennis on the very first day of the grass-court Grand Slam.
More than half the questions at Sunday's media session revolved around themes generating the most buzz on the eve of tennis' oldest and most prestigious Grand Slam tournament: what Williams was quoted as saying in a recent magazine article — and Sharapova's surprisingly forceful verbal swipe in reaction to that story.
Williams reached the French Open final for the first time since 2002 when she beat Sara Errani 6-0, 6-1 Thursday. The 15-time Grand Slam champion won her only Roland Garros title 11 years ago, beating sister Venus in the final.
Djokovic, the winner of six major titles, seeks to become the eighth man to complete a career Grand Slam, but he'll have to get past seven-time French Open champion Nadal first.