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The hosts, which began the day at 34-2 in its second innings, went to lunch on 96-7 and an overall lead of 162.
Veteran left-hander Shivnarine Chanderpaul was unbeaten on 12 off 57 balls with captain Darren Sammy on 7 not out. Lendl Simmons top-scored with 21.
Ajmal followed up a five-wicket haul in the first innings with another superb performance on a difficult pitch.
Ajmal, who had claimed the wicket of Darren Bravo late on Friday, added the scalps of nightwatchman Kemar Roach, Ramnaresh Sarwan and Carlton Baugh.
Roach fell off the day’s sixth delivery when he was trapped lbw on the back foot.
Left-arm seamer Wahab Riaz made a crucial breakthrough soon afterwards when Simmons chipped a catch to short leg, where Azhar Ali clutched a sharp, chest-high chance on the second attempt.
Wickets continued to tumble as Sarwan gloved a sharp turner to short leg off Ajmal.
The hosts gifted Pakistan another wicket when Brendan Nash was run out after he tumbled, trying to abort a second run after being sent back by Chanderpaul.
Ajmal rounded out a fine session for the visitors when he claimed Baugh as he dragged a catch to midwicket at 86-7.
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