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May had previously been in touch with Brussels only by text message since Tuesday, when the British parliament rejected the divorce deal she signed in November.
“Discussed with PM @theresa_may the next steps on the UK side. #Brexit,” tweeted Tusk, who represents EU leaders as president of the European Council.
May also spoke separately with the head of the EU executive, European Commission president Jean-Claude Juncker, at her request.
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British politicians are wrangling over how to get out of the Brexit impasse, which could see Britain crash out of the union without a deal on March 29.
EU leaders have so far ruled out renegotiating the agreement, but have signalled they could postpone the withdrawal if May comes up with a plan.