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Despite the worries of casting someone who is better known as a singer in the role, director Yoon Sung-sik decided to cast IU after seeing her performance in Dream High and thought that she suited the image he had envisioned for the character.She was nominated for the Excellence in Acting Award (Best Actress in a Serial Drama) at the 2013 KBS Drama Awards.2011 also saw her first foray into song-writing with "Hold My Hand", which was written for the television series The Greatest Love.IU's third full-length album release, Modern Times (2013), showcased a more mature style that was a departure from her established girlish image, with several tracks reaching the top 10 positions on Gaon Digital Chart.On March 10, 2011, IU performed as the opening act for British singer-songwriter Corinne Bailey Rae's first solo concert in Seoul with two songs, before joining Bailey Rae during her performance of "Put Your Records On".The Korea Joong Ang Daily described the album as one that would "suit all kinds of musical tastes and fans", while Billboard noted the "cinematic feel" of the album as set by the opening track, "Secret" (Korean: Produced by Jo Yeong-cheol, whom IU worked with on Real, the album contains collaborative works with singer-songwriters such as Yoon Sang, Lee Juck and Ra. The total number of download sales made from the album's tracks exceeded 10 million within the first two weeks.
Almost two years after Last Fantasy, IU released her third studio album, Modern Times, on October 8, 2013.
She also collaborated with artists such as Mighty Mouth and The Three Views on their albums.
As her popularity began to rise, IU made more frequent appearances on variety shows, performing on Star Golden Bell, Kim Jung-eun's Chocolate and You Hee-yeol's Sketchbook.
Admitting that she was doubtful about her readiness to take on acting, IU remarked that she gained confidence in learning that the part would require singing and would later describe the experience as a tremendously enjoyable one.
IU took on various side-projects after the end of Dream High.