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India were all out for 286 in their second innings on the third day of the match.
Enjoying a brilliant all-round outing on a surface that has tested the skill and temperament of the best of batsmen from both sides, seasoned off-spinner Ashwin showed how to do it with his excellent knock of 106 off 148 balls.
Captain Virat Kohli struck 62 off 149 balls and added 96 runs for the seventh wicket with Ashwin, helping India extend their overall lead after they were reduced to 106 for six at one stage.
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Kohli struck seven boundaries during his stay in the middle while Ashwin found the fence 14 times and cleared it once at the MA Chidambaram Stadium.
For the visitors, senior spinner Moeen Ali registered impressive figures of 4/98, while Jake Leach picked up 4/100.
Brief Scores:
England 1st Innings: 134 all out
India: 329 and 286 all out in 86.5 overs (Virat Kohli 62, Ravichandran Ashwin 106; Moeen Ali 4/98, Jack Leach 4/100).