Pendulum once again toured Europe in 2009. During this tour they announced that they were working on their third studio album, Immersion. It was announced in December 2009 that Pendulum would be touring for their new album in May 2010. The release date of the album was announced to be sometime "in May" during the live preview party at Matter, and was then announced to be released on 24 May. Pendulum previewed their album Immersion at the Ear Storm night at London's Matter nightclub on Friday 22 January. "Salt in the Wounds", a track from their new album, was Zane Lowe's Hottest Record in the World on BBC Radio 1 on 25 January 2010. On Zane Lowe's show, it was also announced that he wanted to join the band and the first single from the new album would be called "Watercolour". This single also received its first play on Zane Lowe's BBC Radio 1 show on 8 March 2010, and was his Single of the Week for that week. In December 2010, "Watercolour" was found to be featured in the soundtrack of the 2010 hit game "Need for Speed: Hot Pursuit". On 1 April, the music video for "Salt in the Wounds" was released. The video is unique in that it is, according to the band's website, "...the world's first 360deg interactive music video."  "Watercolour" claimed the No.4 spot in the UK Singles Chart, making it their biggest hit to date. On 21 May 2010, the band headlined the annual Radio 1's Big Weekend festival which was held at the Vaynol Estate, Bangor, Gwynedd. The second single from the album, "Witchcraft", was released on 18 July and charted at No.29 in the UK Singles chart, making it their third highest charted single in the UK. The third single from Immersion was "The Island", and just missed the UK Top 40 at No. 41.  Rob Swire had stated that if it had achieved greater success than "Witchcraft", he would have released a song entitled "Ransom", which was taken off Immersion before the album's release. Swire revealed the original files for "Ransom" were corrupted, and that he has no plans to recreate them, therefore it will not be released. However, on 6 April 2011, Pendulum released "Ransom" as a single via their website with all proceeds going to the Help for Japan fund after the tsunami. "Crush" was released as the fourth single in January 2011. In January 2011, Pendulum released a Deluxe Edition of Immersion via iTunes which contained the album's original 15 tracks and a collection of remixes of "Watercolour", "Witchcraft" and "The Island" by other artists including deadmau5, Tiesto and Chuckie. Both the UK and US store were also given the music videos of those three tracks in the release.

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