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Larson was one of an initial group of three to roll out in the second and final round of qualifying, laying down an initial 1:28.079s in the #5 Hendrick Motorsports Chevrolet.
Daniel Suarez (#99 Trackhouse Racing Chevrolet) moved into second with a 1:29.230s while Brad Keselowski spun the #6 RFK Racing Ford at Turn 11 but was able to press on.
Michael McDowell (#34 Front Row Motorsports Ford) went to the top with a 1:27.862s in the eighth minute of 10, as Larson headed out for a second run.
Van Gisbergen, who had taken pole position in the Xfinity Series earlier in the day, moved into third place with a 1:28.183s in the #16 Kaulig Racing Chevrolet with just over a minute remaining.
Larson improved to a 1:27.864s in the moments before the chequered flag but it was two thousandths too slow to match McDowell’s provisional pole time.
Ty Gibbs (#54 Joe Gibbs Racing Toyota) then went top with a 1:27.846s and while van Gisbergen was unable to improve on his final lap, Larson dug deep with a 1:27.836s to snatch pole.
He and Gibbs will share the front row tomorrow, ahead of McDowell, Tyler Reddick (#45 23XI Racing Toyota), van Gisbergen, Bubba Wallace (#23 23XI Toyota), Christopher Bell (#20 JGR Toyota), Alex Bowman (#48 Hendrick Chevrolet), Suarez, and Keselowski.
Back in Round 1, van Gisbergen waited until nine minutes into the 15-minute Group A segment to head out and set a 1:28.507s.
That put him fifth and hence right on the bubble but he went to the top with a 1:27.864s next time around, flying in formation with Trackhouse Racing stablemate Daniel Suarez (#99 Chevrolet), who set a 1:28.159s.
A red flag followed when Corey LaJoie (#7 Spire Motorsports Chevrolet) hit the wall at Turn 11, after which Larson moved into top spot with a 1:25.518s which would prove the fastest lap of the stanza.
Van Gisbergen was through in second, ahead of Keselowski, McDowell, and Suarez, with Ross Chastain (#1 Trackhouse Chevrolet) seventh.
In Group B, Gibbs was fastest throughout, advancing along with Bell, Reddick, Wallace, and Bowman.
Harrison Burton spun into the Turn 6 tyre wall with the chequered flag out, causing damage to the #21 Wood Brothers Racing Ford.
Xfinity Race start is scheduled for today at 15:30 ET/05:30 AEST, with the Cup Race kicking off tomorrow at 16:30 ET/06:30 AEST.
