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Let me preface by saying I have never been one with an appreciation for soundtracks.
The few exceptions are typicaly classicaly oriented. That said, run out and buy "Once".
This soundtrack is filled with an aching beauty that elevates these songs beyond "soundtrack".
I think Glen sounds a little like Cat Stevens on the opening "Falling Slowly" with Marketa Irglová singing along clean and sparse. "If you want me" is a haunting call for love. I could do with out "Broken hearted hoover fixer sucker guy", for me it is the one low point on the record. Marketa's"The Hill" is absolutely heartbreaking.
Also worthy of being searched out is "The Swell Season" by Irglová and Hansard from 2006. They just sound so good together.