//display window without any of the usual dressing
[window setStyleMask:NSBorderlessWindowMask];
//set 'z-index' of window to display on top of menubar
[window setLevel:NSMainMenuWindowLevel+1];
//set the window rect to the screen rect
NSRect mainDisplayRect = [[NSScreen mainScreen] frame];
[window setFrame:mainDisplayRect display:YES];
There's more to it than that, but it would help to see where you've got to. This approach eschews the OSX10.7+ fullscreen goodness - as you have probably worked out, it is not easy under these new fullscreen patterns to work with dual monitors. With the above method, you can control an app from one screen (retain menubar, other windows, full access to the OS) whilst playing one of its windows fullscreen on a second monitor.
By the way, the new version of iTunes brings back some dual-monitor functionality. There is a way to set it up so that you have full-screen video on one monitor whilst some degree of controlling (using the miniplayer) on a second screen.