The failure to reach a breakthrough deal, aimed at easing growing international concern over Iran's contested nuclear activity, marked a further setback for diplomatic efforts to resolve the decade-old dispute peacefully.
Underlining the lack of substantial progress during the meeting in the Kazakh city of Almaty, no new negotiations between the two sides appeared to have been scheduled.
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"It became clear that our positions remain far apart," Ashton, who represents the six powers - the United States, Russia, China, France, Britain and Germany - in dealings with Iran, told a news conference.
Russia's negotiator sounded more upbeat, saying the talks were "definitely a step forward" although no compromise had been reached, Interfax news agency reported, without giving details.
Iran's critics accuse it of covertly seeking the means to produce nuclear bombs and say Tehran in the past has used diplomacy as a stalling tactic. Further inconclusive talks will not reassure Israel, which threatens air strikes, if necessary, to stop its arch-enemy from getting the bomb.
The Jewish state is widely believed to have West Asia's only nuclear arsenal. Iran says its nuclear energy program is entirely peaceful but UN inspectors suspect it has worked illicitly on designing a nuclear weapon.
With all sides aware that a breakdown in diplomacy could shunt the protracted stalemate a step closer to war, no one in Almaty was talking about abandoning diplomatic efforts.
Ashton said that for the first time there had been a "real back and forth between us when were able to discuss details, to pose questions, and to get answers directly ... To that extent, that has been a very important element"
But, she added: "What matters in the end is substance. We know what we want to achieve and the challenge is to get real engagement so we can move forward with this and that's the ambition."
With a presidential election due in Iran in June, scope for a breakthrough was slim in Almaty, when Iran declined to accept or reject an offer of modest relief from economic sanctions in exchange for curbing its most sensitive nuclear activity.
Without substantial progress in coming months, Western governments are likely to increase economic sanctions on Iran.
The talks were held against a backdrop of flaring tension between big powers and North Korea, which like Iran is defying international demands to curb its nuclear programme.
But unlike North Korea, which has carried out three nuclear tests since 2006, Iran says its nuclear energy activity is entirely peaceful.
DEADLOCK CONTINUES
| Iran, world powers remain "far apart" - EU foreign policy chief Catherine Ashton
| But Russia sees "step forward" in Almaty talks
| Israel might become increasingly impatient with diplomacy
| Iran denies nuclear weapons aims
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