The fatal shooting will most probably heighten tensions following violent clashes on Friday night between riot police and supporters of the group that injured some 75 people.
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They gave the group until 1300 GMT to lay down their arms and surrender.
Investigators say 23 opposition supporters have been detained following the unrest.
Police spokesman Ashot Agaronyan said on Facebook the policeman was in a vehicle 400 meters (yards) from the station when he was killed by sniper fire.
The gunmen – supporters of fringe jailed opposition leader Zhirair Sefilyan – stormed the police building on July 17, killing one officer, taking several more hostage and seizing a store of weapons.
“Or else, special units of law-enforcement bodies will be authorized to open fire and neutralize, without prior warnings, any armed person in and outside the [seized] police regiment”, Armenia’s National Security Service (NSS) said in a statement issued at 4 p.m. local time.
Three of the gunmen were wounded in Friday’s exchange of gunfire with police, with two taken to hospital under armed guard.
The deadline passed with no immediate action taken.
Journalists, including from Radio Liberty, reported being attacked and beaten by men armed with sticks and metal bars who appeared to be plainclothes police officers. Riot police used tear gas and stun grenades to end the protest organized by politicians and public figures allied to Founding Parliament, a radical opposition group with which the gunmen are affiliated. A senior doctor there told RFE/RL’s Armenian service that majority suffered burns apparently caused by the police flashbangs.
The latest developments in Armenia’s capital Yerevan, related to the seized Erebuni police station, are very worrying. The Prosecutor General’s launch of a criminal case into violence against journalists is a positive initial step, and we call on the government to allow a full, independent, and transparent investigation into all allegations of human rights violations, and to prosecute all those involved to the fullest extent of the law.
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“Use of force and violence to achieve political change are not acceptable”, an European Union spokesman said in a statement.
