"We are in the middle of talks about nuclear proliferation and reining in Iran's programme, it is a really tough negotiation I will tell you," Kerry said during a second day of high-stakes discussions in Vienna.
His talks with Iranian Foreign Minister Mohammad Javad Zarif were in order to "gauge Iran's willingness to make the critical choices it needs to make," a senior US official said.
It was unclear how long they would last, although Egyptian state media reported that Kerry would visit the country tomorrow in an effort to broker a truce in Gaza.
The mooted accord would kill off for good fears that Iran might develop nuclear weapons under the guise of its civilian programme after a decade of rising tensions and threats of war.
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Iran denies seeking the atomic bomb and wants the lifting of crippling UN and Western sanctions.
The five permanent members of the UN Security Council plus Germany have been negotiating almost non-stop for months, after sealing an interim accord in November under which Iran froze its uranium enrichment in return for about USD 7 billion in sanctions relief.
Both sides are also under intense domestic pressure.
Zarif will have to come up with a deal that satisfies Iran's hardline Islamic leaders, while Kerry is under pressure from Congress ahead of November mid-term elections not to concede too much.
Kerry, along with the foreign ministers of France, Germany and Britain and the deputy foreign minister of China jetted into the Austrian capital yesterday seeking to inject some momentum.
Russia sent a lower-ranking official, but Washington dispelled any speculation -- stoked by comments by French Foreign Minister Laurent Fabius last week -- of divisions between the six powers.
"It is now up to Iran to decide to take the path of cooperation... I hope that the days left will be enough to create some reflection in Tehran," Germany's Frank-Walter Steinmeier said.