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"They began to shoot, and with my own eyes I saw how one man was wounded in his leg and another in his arm," she said.
Government troops appeared to have lost an armored personnel carrier to attacking mobs. By nightfall, all government forces had abandoned the city center, which was blocked off with barricades of tires.
U.S. State Department spokeswoman Jen Psaki condemned the violence, which she said was "caused by pro-Russia separatists."
"We continue to call for groups who have jeopardized public order by taking up arms and seizing public buildings in violation of Ukrainian law to disarm and leave the buildings they have seized," she said.
Meanwhile, the Obama administration and NATO Secretary General Anders Fogh Rasmussen condemned Putin's visit to Crimea.
"We still consider Crimea as Ukrainian territory and from my knowledge the Ukrainian authorities haven't invited Putin to visit Crimea, so from that point of view his visit to Crimea is inappropriate," Fogh Rasmussen told reporters in Tallinn, Estonia.
Psaki called the trip "provocative and unnecessary."
Earlier, in Moscow, Putin watched as about 11,000 Russian troops marched across Red Square to the tunes of marches and patriotic songs. They were followed by columns of dozens of tanks and rocket launchers as some 70 combat aircraft, including giant nuclear-capable strategic bombers, roared overhead.
In a dig at Ukraine, the parading troops on Red Square included one marine unit from the Black Sea Fleet that flew the Crimean flag on its armored personnel carriers.
The West and the Ukrainian government accuse Russia of fomenting the unrest in Ukraine's east, where insurgents have seized government buildings in a dozen cities and towns.
The referendum on independence being held Sunday in the Donetsk and Luhansk regions — an area that encompasses 6.5 million people — is similar to the plebiscite that paved the way for Moscow's annexation of Crimea.
Putin's surprise call Wednesday for the rebels to delay the vote appeared to reflect Russia's desire to distance itself from the separatists as it bargains with the West. But insurgents in Ukraine's Russian-speaking east defied Putin's call and said they would go ahead anyway.
Putin also said Russia had withdrawn its forces from the Ukrainian border, but the Pentagon and NATO said there was no evidence of a pullback.
"We still don't have visible evidence of Russian withdrawal of troops from Ukraine's border," Fogh Rasmussen told reporters Friday. "I would be the first to welcome it if Russian troops were pulled out."