After three meetings that Washington says have enabled both sides to "understand each other's positions", the negotiators aim this time to start drafting the actual text of an accord.
Success could resolve one of the most intractable geopolitical problems of the 21st century, but failure could plunge the Middle East into conflict and start a regional nuclear arms race.
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The five permanent members of the UN Security Council plus Germany want Iran to reduce in scope its nuclear programme so as to make any dash to build an atomic bomb virtually impossible.
In return the Islamic republic, which says its nuclear activities are purely peaceful, wants the lifting of all United Nations' and Western sanctions, which have hit its economy hard.
Iran's Foreign Minister Mohammad Javad Zarif, installed by bridge-building new President Hassan Rouhani last year, said after the last round that there was agreement on "50-60%" of issues.
But with both sides sticking to the mantra that "nothing is agreed until everything is agreed" -- one US negotiator likened the process to a "Rubik's Cube" -- this is not enough.
Arriving in Vienna yesterday, both Iran and the United States sought to dampen expectations that a deal was within easy reach, with Zarif saying a "lot of effort" was still required.
A senior US official said the talks would be "very, very difficult" and that there were still "significant gaps" between the two sides and a "range of complicated issues".
"We do not know if Iran will be able to make the tough decisions they must to assure the world that they will not obtain a nuclear weapon and that their programme is for entirely peaceful purposes," the official said.
She added that optimism raised in some quarters has "gotten way out of control".
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