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Equalling his best ever showing at Wimbledon, Daniil Medvedev downed Hungary's Marton Fucsovics 4-6 6-3 6-4 6-4 to reach the fourth round.
Ninth seed Kviotova brushed aside the challenge of Belarusian Aliaksandra Sasnovich.
The left-hander looked completely at ease on the surface as she captured her sixth title on grass, more than any other active Women's Tennis Association player.
By winning her 30th career title, the former world No. 2 Kvitova will now re-enter the top 10 for the first time since September, 2021.
Tsitsipas will next take on Italian Jannik Sinner in what could be a tricky test.
Alcaraz, last year's quarterfinalist, remained on course for another memorable run at Flushing Meadows after squeezing past 2014 champion Cilic to set up a showdown against Jannik Sinner.
World No. 1 Iga Swiatek was made to work by American Lauren Davis before sealing a 6-3, 6-4 win to reach the fourth round at New York for the second straight year.
The US Open draw did Serena no favours, the 40-year-old American landing in the bottom quarter where fifth-seeded Tunisian Ons Jabeur, the Wimbledon runner-up, 10th-seeded Daria Kasatkina and last year's losing finalist Leylah Fernandez all lurk.
After battling through qualifying, Garcia beat three top-10 world-ranked opponents, Maria Sakkari, Aryna Sabalenka and Jessica Pegula, on the way to the final where she delivered a master class against Czech Kvitova.
Petra Kvitova overcame a sluggish start and 10 double faults to beat Madison Keys 6-7(6), 6-4, 6-3 and advance to the women's singles final, where she will face Caroline Garcia, the first qualifier to reach the final of a WTA 1000 tournament.