I have a PHP background. I would like to learn another language to build programs that can be run on Windows. I have my eye on C#.
What I really would like to accomplish is to be able to make programs on Windows that have a better UI then the traditional Windows program generally has. For example, I really like the way Apple/Mac programs look. Apple has iTunes that runs on Windows and looks nothing like a traditional Windows program so I assume it is possible.
So my question, what languages(s) or technologies would you point me towards to accomplish a Windows program that could have a nice UI like the image below instead of the way most Windows programs look?

What languages and technologies would you recommend for building an app that looks like this that can run on Windows?
There are a variety of 3rd part components you can use to spruce up the look and feel of your application. In no order of importance, a few of the big players are:
For which ones people like the best, search SO for opinions. Be forewarned, everyone tends to get a bit religious/devoted to the ones they like.