Danny Alexander has called on Scottish ministers to produce "realistic analysis" of the cost of independence.
It comes as the Treasury prepares to publish detailed findings on the financial impact of a "Yes" vote.
In a speech in Edinburgh on Wednesday, the Chief Secretary to the Treasury will attack "over-optimistic assumptions" about oil revenues.
A spokesman for the first minister said Scotland had the "financial resources to be a successful independent nation".
Mr Alexander's attack on the Scottish government's white paper on independence comes a few weeks before the Treasury's most detailed fiscal analysis is due to be published.
Chancellor George Osborne and Mr Alexander asked the department's economists to calculate "in detail the figures that illustrate the benefits of the UK and the cost of independence".
The UK government said economists had spent months analysing data and forecasts, and consulting with independent bodies.
It said the analysis would set out "in more detail than ever before the impact of having to absorb the higher spending and lower tax caused by declining oil revenues, an ageing population, the Scottish government's uncosted policy pledges and the set-up costs of independence in a much smaller budget".
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