From October 2009 to January 2010 Vickers played the title role in a West End revival of The Rise and Fall of Little Voice for which she won the award for "London Newcomer of the Year" at the Theatregoers' Choice Awards. Vickers' debut single, "Once", charted at number one on the UK Singles Chart after its release on 19 April 2010 and has sold over 220,000 copies in the United Kingdom. Vickers' debut album was released on 3 May 2010 in the United Kingdom achieving number one status on the UK Albums Chart, number seven on the Irish Albums Chart and number four on the European Top 100 Albums, and has been certified Gold by the BPI. Songs from the Tainted Cherry Tree went on to sell over 300,000 copies in the United Kingdom.
Her second single, "The Boy Who Murdered Love", charted at number 36 on the UK Singles Chart. This was followed by her third single, "My Wicked Heart", which was released on 17 October 2010 digitally and on 1 November 2010 physically. "My Wicked Heart" peaked at number 13 on the UK Singles Chart, making it Vickers' third consecutive Top 40 single. At the end of 2010, Vickers became RCA's highest grossing domestic artist.
In May 2011 Vickers unveiled her debut fashion line for Very.co.uk titled "Dee V" reinforcing her signature quirky fashion sense. Vickers' distinctive and unique boho-chic approach to fashion has achieved industry praise from prestigious fashion magazines including Grazia, Look, and Harpers Bazaar. Vickers is also the face of make-up and cosmetic range, Collection 2000.
On 31 August 2012, it was reported that Vickers had landed her debut film role alongside Clint Eastwood's son. The independent film titled The Perfect Wave is filmed in Cape Town, South Africa where Vickers re-located from London whilst starring in it. Vickers also appears in a forthcoming comedy series titled Give Out Girls for Sky Living, which marks Vickers' debut in television acting.
On 9 April 2013, it was confirmed that the lead single to Vickers' second album is titled "Cinderella", with a preview snippet being made available on iTunes. "Cinderella" was released on 21 July 2013 in the United Kingdom. It broke into the Top 15 of the UK Indie Chart peaking at number 13. Vickers' second album and a single of the same name titled, Music to Make Boys Cry followed on 15 September 2013. Music to Make Boys Cry charted at number 37 on the UK Albums Chart and number 9 on the UK Indie Chart on 22 September 2013.
Vickers sings "My Favourite Things", a classic song from The Sound of Music on the One Direction television advertisement for the launch of their fragrance, Our Moment.
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