Spanish Prime Minister Mariano Rajoy called the vote a "mockery" of democracy, and the European Commission expressed support for Madrid's position before the referendum.
Sunday's vote saw scenes of violence with police charges against voters, with the Spanish Interior Minister claiming 431 law enforcement officers had been injured and Catalan medical services reporting 893 people had needed medical attention after baton charges and the region was paralyzed by a strike on Tuesday in protest at the police actions.
Puigdemont's comments appeared after Spain's King Felipe VI accused secessionist leaders on Tuesday of shattering democratic principles and dividing Catalan society, as tens of thousands protested against a violent police crackdown on Sunday's vote.
In a last-ditch attempt to bring Catalonia back under control European Union officials have warned quitting Spain would also mean quitting the bloc. We don't want a traumatic break. "It's time to talk, to find a way out of the impasse working within the constitutional order of Spain".
The silence of the EU on Madrid's excesses against the Catalan separatists may not bode well for its credibility among Europeans, especially among newly formed fledgling states of the future, like Catalonia.
At this point, all communication channels between the Spanish and the Catalan governments seem to be broken.
During an exclusive visit today to Catalonia's presidential palace, which dates to the 14th century, Catalan leaders met in a chapel without their cellphones, likely out of fear their phones were tapped by Spanish authorities.
Officials estimated voter turnout for Sunday's referendum was about 42.3 percent of 5.34 million eligible voters.
The four include regional police chief officer Josep Lluis Trapero and Jordi Sanchez, the head of the Catalan National Assembly that has been the main civic group behind the independence movement. Spain's conservative government has said it will respond with "all necessary measures" to counter Catalan defiance, and is holding talks with opposition leaders to forge a consensus over what to do in response.
The Venice Commission's secretary general Thomas Markert did make the point of referencing the 2014 Scottish referendum, highlighting it as an example of a fair, legally-approved vote as it gained the support of the United Kingdom government.
Timmermans said the images of clashes between Spanish police and independence activists was "saddening", but defended Madrid's right to use "proportionate" force. "We are under observation day and night", Puigdemont said.
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