The 20-year-old Larcher de Brito, who had shown signs of future promise as a teenager over the last several years but had never quite grabbed that one breakthrough result, finally grabbed it this time, going toe to toe with Sharapova in a high-quality slugfest in front of an electric Court 2 crowd.
The No.3-seeded Sharapova did everything in her power to block a happy ending for Larcher de Brito - she fought off four match points in the last game, including two with huge forehand winners - but one last forehand into the net finally sealed the deal, and Larcher de Brito got that big breakthrough.
"It was a combination of everything," Sharapova said. "I give her a lot of credit. I think she played extremely well. She was really solid from the baseline. I don't feel like I was aggressive enough, that I hit the ball deep enough. I wasn't ready after the returns or serves. I just wasn't there, really."
Sharapova slipped to the court several times during the match, but didn't use it as an excuse. "I don't think I've ever fallen three times in a match before in my career so that was a little strange, but that's certainly not an excuse. I think today I've seen a lot of players fall and take a few hits and a few injuries. I think that's just part of the game, part of what we have to deal with as tennis players."
The second round loss was Sharapova's earliest loss at a Grand Slam since she fell first round at the 2010 Australian Open. "It's frustrating," she said. "You don't want to lose matches, whether it's early or late in the draw, but this tournament is extremely special, so it's especially tough to lose here.
"But I'm going to keep my head high about it because there's no other way. I'll find the positives out of what I have done today and in my career, set new goals, and try to just keep moving forward."
Meanwhile, Larcher de Brito, who already had three Top 20 wins to her name, got her first over a Top 10 player. And what a stage for it too - playing a WTA legend at the most legendary tournament.
"I'm really excited. I really can't believe it. It's a little bit of shock and excitement," Larcher de Brito beamed afterwards. "I'm just really happy I got through that match. It was a really great win for me.
"The end was really nerve-wracking. I tried to stay calm. I gave it my all. It was 5-4. If I lost that, it would have been 5-all. If it were 5-all, it would have been tough to get back up again, because she was serving, and she was serving really well. I thought, 'Now or never.' I tried to stay calm, even though it's hard sometimes. I just gave it my all, like I always do, and it turned out well for me in the end."
Larcher de Brito has been talked about for years now - at age 14 in 2007 she became one of the Top 10 youngest players ever to win a WTA main draw match, in 2009 she cracked the Top 100, and things seemed on the up and up. But she comes into Wimbledon at No.131 - it hasn't been a smooth ride.
"When I was 16, when I was in the Top 100, everybody was comparing me to like Martina Hingis, and expecting me to win a Grand Slam at that age. But that doesn't happen anymore, winning Grand Slams so young. Tennis is such a competitive sport now and so hard, it's just really hard to stay there.
"But I just tried to keep going, and now I'm here again, and I hope to keep doing well all year."
The Portuguese pointed to two people in particular who helped keep her going in the sport.
"I wouldn't be here if it wasn't for my parents," she said. "I'm not one of those players who is going to make up excuses like I was sick or injured, none of that. I simply wasn't playing well. I had no motivation. I'm just lucky I had my parents next to me, supporting me, helping me to keep going. It was really tough for me at one stage. The only people I had left was my mom, my dad, my brothers. They were supporting me through this really tough time. Now they're still here with me when I'm succeeding.
"I'm not going to lie. I did drop off the radar a little bit. That's just why it makes the wins that much more sweeter. I'm really grateful to have a wonderful family that supported me all these years."