One of the first Calvinist authors I read thoroughly was Jonathan Edwards. He was much derided in my high school American Lit class for the hellfire of "Sinners in the Hands of an Angry God", but he wrote hundreds of other books and sermons as well. His Freedom of the Will is an epic logical tome of metaphysics, in which it is explained that we do things because of our nature, and our wills are bound to that nature. In Calvinist speak this deals with the Sovereignty of God and the depravity of man. Despite the fact of our moral instincts, there are sociopaths who lack this instinct on one hand, and on the other none of us complies with our instinctual morals perfectly (white lies, outbursts of rage in an otherwise gentle soul, etc.)

But neuroscience shows that things we do are a product of biology, chemistry, physics. I have some disagreements with Sam Harris, but this area in particular is his expertise.