Going into a second day of negotiations in Vienna with foreign minister Mohammad Javad Zarif, Kerry aimed to "gauge Iran's willingness to make the critical choices it needs to make," a senior US official said.
"That's a pretty serious and potentially lengthy conversation. The secretary will take the time necessary to have that discussion," the official said.
"I am glad that we can have some time to be able to catch up and pick up where we left off," said Kerry.
Zarif appeared to be in for the long haul too, telling Iranian media on Sunday there were still "seven difficult and tough days for discussion".
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.
Iran denies seeking the atomic bomb and wants the lifting of all UN and Western sanctions, which have crippled its economy.
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 $7 billion in sanctions relief.
But the talks to nail down a full treaty have met major sticking points, particularly on how much of Iran's nuclear programme to dismantle.
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.
The United States and Iran have not had diplomatic ties for three decades, making the face-to-face talks between the two top diplomats all the more remarkable.
On Sunday Kerry, the foreign ministers of France, Germany and Britain and the deputy foreign minister of China jetted into the Austrian capital seeking to inject some momentum.
Russia sent a lower-ranking official, but Washington dispelled any speculation — sparked by comments by French Foreign Minister Laurent Fabius last week — of divisions.
But the three European ministers left with no apparent breakthrough. "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.
"The ball is in Iran's court." Britain's foreign secretary William Hague said it was "very important for Iran to be more realistic".
Before leaving Vienna, Hague said there had been no "decisive breakthrough" and a "huge gap" remained on the key issue of uranium enrichment.
This activity can produce fuel for the country's sole nuclear plant or, if further enriched, the material for an atomic bomb.
The six powers want Iran to reduce dramatically the scope of its enrichment programme, while Tehran wants to expand it.
Israel, the Middle East's sole if undeclared nuclear armed state and which together with Washington has refused to rule out military action, is opposed to any enrichment by Iran.
Israeli Prime Minister Benjamin Netanyahu warned Sunday that any nuclear deal leaving Iran with the capability to pursue this activity would be "catastrophic".
Iranian negotiator Abbas Araqchi was on Sunday publicly sticking by Iran's position on enrichment which he called "clear and rational".
"As the supreme guide said, the enrichment programme has been planned with the real needs of the country in mind, meaning our need to ensure reactor fuel."
If no agreement is reached by Sunday when the six-month interim accord runs out, all sides can agree to extend the talks for a further six months.
Hague said on Sunday that such a move "will only be discussed if no progress can be made. It is still too early."
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