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On October 27, 2007, Rossum again sang the national anthem at the New Jersey Devils's first home game of the 2007–08 NHL season, which was also the first game the team played in the newly constructed Prudential Center.
She also performed at the Hollywood Christmas Celebration at the Grove in Los Angeles In 2010, Rossum sang a song called "Cruel One" on singer Alex Band's debut solo album We've All Been There. Records album Sentimental Journey on January 29, 2013.
She also had a guest role as Caroline Beels in Snoops.
Rossum was nominated for a Young Artist Award in 1999 for Best Performance in a TV Movie for her work in the made-for-TV movie, Genius.
After her role in The Phantom of the Opera, Rossum was offered several deals to record classical albums, but refused, opting to create an album of contemporary, more mainstream music.
"I was inspired to cut this album because I'm so frustrated listening to the radio these days," Rossum lamented.
Rossum had a breakthrough role as Laura Chapman in the Roland Emmerich eco-disaster film The Day After Tomorrow (2004).
She later returned to New York, where she was the last to audition, in full costume and make-up, for the role of Christine Daaé in The Phantom of the Opera (2004), the onscreen adaptation of composer Andrew Lloyd Webber's musical of the same name.
Debuting at the Sundance Film Festival, the film won the Special Jury Award for Outstanding Ensemble Performance.
Rossum described the character as being proactive and strong in all situations, rather than a damsel in distress.
In November 2009, Rossum appeared in Broadway's 24 Hour Plays in which actors, writers, and directors collaborate to produce, and perform six one-act plays within 24 hours to benefit the Urban Arts Partnership.
In December 2007, Rossum released three Christmas songs on the EP Carol of the Bells.
It was also this year that Rossum sang the national anthem at the Toyota/Save Mart 350 NASCAR NEXTEL Cup Series race at Infineon Raceway and performed at the first ever Perez Hilton Presents event at the El Rey Theatre in Hollywood.