I would recommend brushing up on your non-frameworked javascript first. Refreshing/learning basic concepts of dom manipulation and what not. Like learning how to build a linked list, stack or queue in C++ before learning how to use the STL (standard template libraries).
In addition to brushing up on straight javascript, it might be good to get into a framework that doesn't abstract and change the way things work so much, for instance Prototype. You code with it very much the same way you code with straight javascript. Read through the Prototype code, learn how to make classes, and do some fancy stuff. From experience, I can say reading through the Prototype.js helped me learn alot.
After messing around a bit, then I'd say go for jQuery. If jQuery didn't, literally, change the way you write code I'd say go for it first, but learning how to build classes and js inheritance and what not can be a very important lesson for someone who wants to become fluent in JS.