“His devotion to Scotland drove his decades of public service.
“We extend our deep condolences to his family and loved ones at this time.”
Mr Salmond had made a speech at the Institute for Cultural Diplomacy Forum and is understood to have collapsed at lunch in a crowded room.
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The Alba party said it understood he had suffered a heart attack, although there will be a post-mortem examination to confirm the cause of death.
Tributes praised him for his decades in politics and efforts to move Scotland closer to independence.
Scotland‘s First Minister and SNP leader John Swinney said he “took the Scottish National Party from the fringes of Scottish politics into government and led Scotland so close to becoming an independent country”.
Sir Keir Starmer called Mr Salmond a “monumental figure of Scottish and UK politics” for more than 30 years who “leaves behind a lasting legacy”.
The prime minister said: “As first minister of Scotland he cared deeply about Scotland’s heritage, history and culture, as well as the communities he represented as MP and MSP over many years of service.”
His former colleague Nicola Sturgeon acknowledged the “breakdown” of her relationship with Mr Salmond but praised him for taking Scotland to the “brink of independence”.
“He was my mentor, and for more than a decade we formed one of the most successful partnerships in UK politics,” she wrote.
Kenny MacAskill, Alba’s deputy leader, said the party “grieves the loss of their founder and leader” but that “the dream he cherished so closely and came so close to delivering will never die”.
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1990: Salmond victory speech
Mr Salmond served as first minister of Scotland from 2007 to 2014 and was leader of the SNP on two occasions, from 1990 to 2000 and from 2004 to 2014.
He resigned as first minister after the 2014 Scottish independence referendum resulted in a 55% to 45% vote to stay in the UK.
He launched his rival Scottish independence party, Alba, in 2021 after his relationship with his successor Nicola Sturgeon fractured.
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