"Talks are underway with the hostage-takers. We are doing our best to resolve the situation without bloodshed," Armenia's first deputy police chief Hunan Pogosyan told AFP.
Lines of police in flak jackets and helmets gathered outside the building Tuesday as parked trucks blocked off surrounding streets, an AFP photographer said.
The gunmen, who captured a large arsenal of police weapons, have so far refused to surrender.
They freed four hostages on Sunday and yesterday, but were still holding four hostages as of today morning, Armenia's national security service said.
The attackers have demanded the resignation of President Serzh Sarkisian and the release of detained opposition leader Zhirair Sefilyan.
More than 1,500 anti-government protesters rallied in Yerevan yesterday, calling for a peaceful resolution to the crisis.
Sefilyan - the leader of small opposition group the New Armenia Public Salvation Front - and six of his supporters were arrested in June after authorities said they were preparing to seize government buildings and telecoms facilities in Yerevan.
A fierce critic of the government, he was arrested in 2006 over calls for "a violent overthrow of the government" and jailed for 18 months. He was released in 2008.
Sarkisian, a former military officer, has been president of the tiny country of 2.9 million people since winning a vote in 2008 that saw bloody clashes between police and supporters of the defeated opposition candidate in which 10 people died.
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