So my solution was to take the magnitude and use that for the 'C' input for surf...
i.e. (psi2 defines the probability distribution function, and mag_R is my magnitude) R = psi2.*sin(theta); X = R.*cos(phi); Y = R.*sin(phi); Z = psi2.*cos(theta); mag_R=sqrt(X.^2+Y.^2+Z.^2);
I then used:
surf(X,Y,Z,mag_R,'EdgeColor','none','FaceColor','interp')
to create the surface I desired.
Thanks for spending your time writing that up for me Walter!