Started to do this last night, then decided I didn’t have my thoughts well enough organized.  Here goes.
Randy & Frylock:  Not sure what else I can say.  Will’s brain wrote Hamlet.  It looks like a volitional act to me, neither random nor determined.
Frylock II:  Regarding #202, sort of but not really.  What I’m saying is that I don’t have to understand how the brain works to observe what it does.  We can observe gravity with great accuracy, yet don’t have a clue how it works.  We can observe volition, albeit with less accuracy, but not knowing how it works is irrelevant to whether it exists.  BTW, I submit that the microscopic level for purposes of this discussion is neurons, not atoms.
Lumpy:  I think everyone agrees that whatever  is happening is happening in the brain.  This has been understood for millennia.  As for your question, there are drugs, as I mentioned above, which improve, for example, impulse control.  I take this as evidence of volition, not the other way 'round.
DSeid:  Grossberg sounds like an interesting fellow.  But so many papers.  Please direct me to two or three which give a nice overview of his theory.
dropzone:  Or, at least, don’t get taken very seriously.
RaftPeople:  You have it backwards.  If theory conflicts with observation, it’s theory which yields.  If volition is real (or, more importantly, is a useful model) and is neither random nor deterministic, then a third category must be constructed.  Maybe algorithmic (influenced by the code, but not deterministically).  But you can’t make volition an illusion by declaring by fiat that there are only two.  Conversely, my position is not dependent on volition being nondeterministic.  Some have argued, e.g., Daniel Dennett, that volition is compatible with determinism.  (But, in a way very different from Hume’s.)  I don’t find the argument persuasive, but not because I’m wedded to nondeterminism.  Rather, it’s simply that I think he’s describing a third category.  Show me he’s right, or show me a similar model which fits, and I’ll happily agree.  It’s volition I care about, not nondeterminism.