Some 37 per cent of those surveyed said they supported independence, with 44 per cent opposed and 19 per cent undecided. This is a five point gain for the "Yes" campaign since the last ICM survey was conducted last September.
"Once the 'Don't Knows' are excluded from the calculation, those figures translate into 46 per cent Yes, 54 per cent No, the highest Yes proportion yet in any poll, other than in a much-criticised poll conducted by Panelbase for the SNP (Scottish National Party) in August last year," explained poll expert John Curtice.
But the survey was criticised as being partisan and the methodology questioned by experts.
Blair Jenkins, chief executive of Yes Scotland, said the new poll "demonstrates very clearly that we are getting our message across and that momentum is very much on our side".
Scots will vote on their independence on September 18 this year.
Scotland has enjoyed increased autonomy within the United Kingdom, which also includes England, Wales and Northern Ireland, since a 1997 referendum.
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