The accused, Head Constable Vijay Prathap Singh (45), allegedly opened fire with a 9mm carbine and killed Assistant Sub-Inspector Ganesan and head constables Subburaj and Mohansingh at the CRPF barracks in Kalpakkam township, about 10 km away from the nuclear complex, according to police.
Operations at the nuclear complex were not affected, officials said.
The incident occurred at the CISF barracks in Kalpakkam township when the troops were gathering for a morning roll call and it was not clear what provoked the attack.
Assistant Sub-Inspector Prathap Singh and head constable Govardhan Singh sustained major injuries and are being being treated at a hospital, police said.
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"This is a disconcerting incident which has happened after a long time in our force. Senior officers have been rushed to the unit and we are cooperating in the police investigation," Central Industrial Security Force Director General Arvind Ranjan said in Delhi.
Singh, a native of Allahabad in Uttar Pradesh, has been arrested and is being questioned by the police.