I really like all of the New Pornographers' output, you really cannot go wrong if you were to choose only one of their albums to spin. That being said, I think Twin Cinema is a really, really great power pop album. For me, Sing Me Spanish Techno is the focal point of that album. It's an incredibly catchy, driving pop song with great singalong-ability. If you have heard the song, then chances are you know what I'm talking about (and possibly agree with me). If you haven't heard it, I honestly think you're missing out and you can give it a chance here.
The New Pornographers > Sing Me Spanish Techno