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Undecided voters in the independence referendum have moved to Yes at a rate of two to one compared with those who have shifted to No, according to Yes Scotland research.
But Better Together say the arguments for keeping Scotland in the UK have changed in recent months with the cross-party offer of more powers if Scotland votes No.
Both sides have pledged to up their game as the 100 day countdown to the referendum begins today.
Yes Scotland leader Blair Jenkins said independence is "a prize that that we must do everything in our power to secure for the people of Scotland''.
Better Together leader Alistair Darling said "the nationalists are running out of arguments - and they are running out of time''.
Mr Jenkins unveiled Yes Scotland research that shows for every 10 people who have moved from the undecided since the autumn, seven have become Yes voters while three have shifted to No.
He said: "I know there are many people who remain to be convinced and it is by talking with them in millions of conversations that we will win them over to Yes.
"Over the next 100 days I appeal to every single person who believes in Yes to make it their business to talk with and persuade those who remain undecided to come our way.''
A hundred Yes Scotland volunteers formed a "gigantic human Yes'' in Edinburgh and displayed 100 arguments for voting for independence ahead of today's milestone.
Mr Jenkins will join SNP deputy leader Nicola Sturgeon and volunteers to unveil a new independence initiative at Dynamic Earth in Edinburgh this morning.
Mr Darling is taking his message around the country today with a series of engagements in Glasgow, Edinburgh and Stornoway in Shetland.
Scotland faces a choice between two competing Scottish visions of the future, according to Mr Darling.
"Something fundamental has changed in that choice since I launched our campaign two years ago,'' he said.
"At that time some of those who were still undecided saw the referendum as a choice between change and the status quo.
"Now - with 100 days to go - the terms of trade have changed.
"And with it the ground has shifted under - and against - our nationalist opponents.
"For it is now clear that a No vote will bring more powers to Scotland within the UK.
"Last week, the Scottish Conservatives produced their proposals for the enhanced powers of the Scottish Parliament.
"All three main Scottish parties backing a No vote now have broadly similar proposals in place.
"There is much that divides us on other issues. But on the constitution - the framework within which legislation is made - we are all now pretty much on the same page.
"I want every voter to understand that within the United Kingdom change and progress is coming to Scotland, under-pinned by the commitments of all three parties.
"We will be offering the guarantee of a constitutional future for Scotland which corresponds with what the great majority of Scots have told us they want.''
Meanwhile, Shadow Scottish Secretary Margaret Curran will address the GMB Congress as the trade union reaffirms its support for a No vote.
She will say that Alex Salmond's "plans for a corporation tax cut and his refusal to back a 50p tax rate show where his real priorities lie''.
"The SNP's first action for our economy would be to hand money back from the Scottish Government to big business,'' she is expected to say.
"They would take money that could fund our schools, our colleges or our hospitals. And send it back to those with the deepest pockets.
"Congress, if you need to know anything about the SNP's priorities for separation I say look no further.''