In general, it's not a good idea to mess with anything inside there. If you did, and then later you wanted to add, change, update, or remove one of those programs - you'd no longer be able to do so.
If the program no longer is installed at all, however, then the point is moot. But you'd be hard pressed to figure out exactly which files in there belong to that program and not shared or used by other programs.
You might try an actual cleanup tool like CCleaner, or even running the built-in "Cleanup Manager" that's part of Windows. To run that, type "cleanmgr" in your Start menu's search box. When it opens, click the "clean up system files" button to make sure it is scanning the global folders like that one (and not just your personal account).