Here's a link to my GITHUB where you will find 'Tiny', a prototype Moodle theme, that I built using Twitter Bootstrap, which, for building a website, is totally awesome. Building a theme for Moodle is hard work, the Bootstrap however makes life a bit easier as all the spade work is done. All you have to do is put all the various componants together and try and blend it in to fit into Moodle.
All I can say is that it's a big, big, big, learning curve...but fun.
Just a note of caution, don't collapse any of your blocks, as they will just vanish into oblivion! If you do lose any checkout another theme and you'll find them again.