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The 24-year-old Pujara scored an unbeaten 206 and batted for close to nine hours before the hosts declared the first innings at 521 for eight shortly after the tea break on the second day and then reduced the visitors to a precarious 41 for 3 at stumps.
Captain Alastair Cook (22) and Kevin Pietersen (6) were the two unbeaten batsmen at close with England still needing 281 runs to avoid the follow on. Nick Compton (9), James Anderson (2) and Jonathan Trott (0) are the three batsmen back in the pavilion on a Sardar Patel track which has already started taking turn.
It was Pujara who hogged the limelight as he not only recorded his second Test century in his sixth match but showed his class with some glorious shots on both sides of the wicket.
The left-handed Yuvraj Singh, playing his first Test since recovering from a rare germ cell cancer, was the other notable performer with a fluent 74 while captain Mahendra Singh Dhoni (5) and R Ashwin (23) and Zaheer Khan (7) could not hang around for long.
Off-spinner Graeme Swann was the pick of the English bowlers with figures of 51-8-144-5, recording his 14th five wicket haul in an innings.
Pujara became only the sixth Indian batsman to hit a double century against England. He joined the list of Mansur Ali Khan Pataudi, Sunil Gavaskar, Gundappa Viswanath, Vinod Kambli and Rahul Dravid.
Pujara batted for a marathon 513 minutes, faced 389 balls and struck 21 fours during his epic unbeaten knock which served as the foundation for India's monumental total.
Off-spinner R Ashwin, who opened the bowling, scalped two wickets and in the process became the fastest Indian to claim 50 Test wickets in his ninth Test, eclipsing Anil Kumble's record of achieving the feat in his tenth match.
The Rajkot-born Pujara took two singles in the 9 balls he faced this morning to reach his first landmark after 16 minutes into the day and then continued to bat with a lot of resolute.
He added 130 runs in 183 minutes for the fifth wicket with Yuvraj Singh, who scored 74 as the two batsmen denied England any wicket in the first session. The duo had come together late last evening and remained unconquered with 98 and 24 in an overnight total of 323 for 4.
India lost the wickets of Yuvraj Singh soon after lunch and also the wicket of captain Mahendra Singh Dhoni, both of them falling to spin bowling.
Yuvraj, not out 72 at the end of session one, could add only two runs in under ten minutes before slogging a full-toss from left-arm spinner Samit Patel straight down to long on fielder Graeme Swann, England's most successful bowler in the innings with figures of 5 for 144.
The 30-year-old left hander, coming back to play his 38th Test match after having survived a rare germ cell cancer batted for just over three hours and hit six fours and two sixes while facing 151 balls. It was his 11th half century in Test cricket.
The partnership for the fifth wicket between Yuvraj and Pujara, that started late last evening and proceeded beyond the first session today, yielded 130 runs in 183 minutes and came off 285 balls.
Skipper Dhoni lasted for 39 minutes while scoring 5 before getting bowled trying a wild sweep shot off Swann. This was Swann's 14th five-wicket haul in 47 Test matches.
Ashwin and Pujara then put on 66 runs for the 7th wicket in 81 minutes before Kevin Pietersen got rid off the former.
After Zaheer Khan fell cheaply to Anderson, the only wicket to fall to a medium pacer, the hosts declared the innings with Pujara unconquered along with Pragyan Ojha.
England commenced their reply late in the evening and India began the proceedings with Ashwin and Zaheer Khan. The off-spinner was shifted to the end from which the left-arm pacer bowled after a four-over spell while Ojha came on from his end.
Ashwin struck almost immediately by making a ball sneak through between the bat and pad of Compton to disturb the stumps. It was also the burly Tamil Nadu off-spinner's 50th wicket in his 9th Test, that made him the fastest among the Indians to reach the landmark surpassing Anil Kumble who had done so in 10 Tests.
In the very next over, Ojha dismissed Anderson as Gautam Gambhir at short leg took a brilliant bat-pad catch to dismiss the left-hander. Ashwin struck another big blow by packing off Trott for a blob, through another catch in the leg trap.
England had lost these three wickets in 13 balls before Cook and Pietersen with Dhoni beefing up the close-in catching positions with four fielders.
In the morning, the home team added 83 runs in 31 overs to their overnight score of 323 for 4 without losing any wicket.
Pujara was unconquered on 133 after having batted for nearly six sessions from just after lunch yesterday while Yuvraj was unbeaten on 72 after a stay of 174 minutes. The Saurashtra youngster needing just two runs to reach his second 100 in only his 6th Test after starting the day at his individual score of 98, got them in singles to long leg in 9 balls that he faced in the morning to complete the landmark in little over four hours and off 190 balls. It was laced with 13 fours.
Yuvraj today added 26 runs to complete his 50 after the first hour of play with a four off Swann.
The pair also completed their century partnership for the fifth wicket in 204 balls and 137 minutes, to pile on more agony on the visitors.