Well, you can pretty much write off VB and ASP (classic). VB still sort of exists (for new development) in the form of VBA, but VB and ASP are legacy tech that are pretty much useless outside of the world of soul-sucking cubicle farms living on the remains of Windows XP. C++ is used where it's used, but that's a shrinking world, if skills-in-demand is what you're after. It's mostly a toolmakers' language now; it's neither small enough for embedded or RAD enough for production. PHP, while ubiquitous, is a crowded space mostly geared towards bending various CMSs to your will. And Java proper tends to be the province of "enterprise" development; none of the cool kids are doing much with the language, even if they're all over the JVM.
If you want to raise eyebrows among potential employers, then learn you a Haskell for great good. Or OCaml. It's not that anybody is using either in anger very much, but they'll mark you as somebody who isn't just following the easiest path to the Land of Promised Jobs. For a less-obviously resume-oriented approach, grab a Scheme (MIT, Racket and Chicken are all good) and work your way through SICP. (And make sure you watch the videos. Watch the videos even if you don't ever touch Scheme or read SICP. There's some head-asplodeeng stuff in there if you've never been exposed to a functional homoiconic language, and it will change the way you think about programming.)