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The duo shared the wickets to reduce Pakistan to 212 for five at the close, a lead of 167 runs, on a Ferozshah Kotla pitch where the ball did not keep as low as on the first two days.
Pakistan would have been in more trouble but for Misbah-ul Haq, who top-scored with 82 in the first innings, being reprieved on one.
He was 29 not out and had raised 51 runs for the sixth wicket with Kamran Akmal, who was on 21.
Pakistan wiped out India's 45-run first innings lead after openers Salman Butt (67) and Yasir Hameed (36) added 71 runs together.
Kumble removed Hameed, Younis Khan (23) and Butt. Harbhajan at the other end struck with his first delivery to send back the experienced Mohammad Yousuf (18) and skipper Shoaib Malik (11), both failing for a second time in the game.
Pakistan leg spinner Danish Kaneria had grabbed four for 59 and debutant left-arm pacer Sohail Tanvir three for 83 to remove the last four Indian batsmen adding 48 runs to their overnight score.
VVS Laxman was undefeated on a fluent 72 but Kaneria took three wickets in 15 deliveries at the other end and the last four wickets fell for 14 runs.
India were bowled out for 276 replying to Pakistan's first innings 231 all out.
Kumble, who claimed four Pakistan first innings wickets, took his tally to seven on his Test captaincy debut at the venue where he took all 10 Pakistan second innings scalps to seal a win in 1999.
The 37-year-old had Hameed caught at silly mid-off playing defensively before Pakistan took tea on 108 for one.
He struck again in the third over of his fresh spell when he trapped Younis leg before and then Harbhajan struck with his first delivery when Yousuf drove back a simple catch.
Butt completed his fifth test fifty with wristy drives and flicks when Kumble forced him to edge a drive to slip. He hit 11 fours in his 140-ball effort spanning 217 minutes.
Six runs later Malik, out for nought in the first innings, chopped an expansive cut against Harbhajan off his boot and on to the stumps to make it 161 for five.
Kumble was unlucky not to remove Misbah, batting at number seven after keeping off the field due to fever, the next over but Wasim Jaffer dropped an easy bat-pad catch at forward short leg.
Misbah went on to hit two sixes to ease the pressure.
The last two Tests will be played in Kolkata and Bangalore.
Pakistan would have been in more trouble but for Misbah-ul Haq, who top-scored with 82 in the first innings, being reprieved on one.
He was 29 not out and had raised 51 runs for the sixth wicket with Kamran Akmal, who was on 21.
Pakistan wiped out India's 45-run first innings lead after openers Salman Butt (67) and Yasir Hameed (36) added 71 runs together.
Kumble removed Hameed, Younis Khan (23) and Butt. Harbhajan at the other end struck with his first delivery to send back the experienced Mohammad Yousuf (18) and skipper Shoaib Malik (11), both failing for a second time in the game.
Pakistan leg spinner Danish Kaneria had grabbed four for 59 and debutant left-arm pacer Sohail Tanvir three for 83 to remove the last four Indian batsmen adding 48 runs to their overnight score.
VVS Laxman was undefeated on a fluent 72 but Kaneria took three wickets in 15 deliveries at the other end and the last four wickets fell for 14 runs.
India were bowled out for 276 replying to Pakistan's first innings 231 all out.
Kumble, who claimed four Pakistan first innings wickets, took his tally to seven on his Test captaincy debut at the venue where he took all 10 Pakistan second innings scalps to seal a win in 1999.
The 37-year-old had Hameed caught at silly mid-off playing defensively before Pakistan took tea on 108 for one.
He struck again in the third over of his fresh spell when he trapped Younis leg before and then Harbhajan struck with his first delivery when Yousuf drove back a simple catch.
Butt completed his fifth test fifty with wristy drives and flicks when Kumble forced him to edge a drive to slip. He hit 11 fours in his 140-ball effort spanning 217 minutes.
Six runs later Malik, out for nought in the first innings, chopped an expansive cut against Harbhajan off his boot and on to the stumps to make it 161 for five.
Kumble was unlucky not to remove Misbah, batting at number seven after keeping off the field due to fever, the next over but Wasim Jaffer dropped an easy bat-pad catch at forward short leg.
Misbah went on to hit two sixes to ease the pressure.
The last two Tests will be played in Kolkata and Bangalore.