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She came to the attention of Neon Gold Records' Derek Davies in 2008, which managed her for six months, and was hired as the supporting act for Australian recording artist Gotye.
At the start of her career, Diamandis was compared to other British female singer-songwriters, with Paul Lester from The Guardian writing that she had a "zeitgeist-y female essence", although she took exception at such comparisons and said that all she shared with Kate Nash was "a vagina and a keyboard." Rory Cashin of Slate lauded Diamandis's lyrics as "esoteric," likening her to an "emotionally intelligent outsider who knew how to perfectly articulate those weird thoughts and reactions we all have but would never admit to." As part of Selfridges' "Sound of Music", Diamandis and Paloma Faith designed their own window display for the London Oxford Street branch in May 2010, and additionally appeared as "live mannequins" for the display.
Her follow-up record Electra Heart (2012) is a concept album about a character of the same name.
It integrates elements of electropop, and its producers include Star Gate, Dr. It became her first number-one project in the UK, where it was also certified gold, and its lead single "Primadonna" is her highest-charting track in the UK Singles Chart, reaching number 11.
In 2009, Diamandis came to prominence upon placing second in the BBC's Sound of 2010.
Her debut studio album, The Family Jewels (2010), incorporates indie pop and new wave musical styles.