In elementary terms, whether the solution to the BVP with boundary conditions given in terms of operators $L_a[f]$ and $L_b[f]$ is guaranteed to exist uniquely comes down to whether the matrix
$$\begin{bmatrix} L_a[f_1] & L_a[f_2] \\
L_b[f_1] & L_b[f_2] \end{bmatrix}$$
is invertible or not, where $f_1,f_2$ are two linearly independent solutions to the homogeneous equation. If it's invertible, then if a solution exists then it is unique, and it turns out that for a "typical" operator the solution exists as well (although this part is more complicated to show in general). If it's singular, then the solution either doesn't exist or isn't unique, and which case you are in depends on what $f$ is.
In the special case of $Lu=u''$, you can choose $f_1=1,f_2=x$. In the pure Dirichlet case there is no problem as you have
$$\begin{bmatrix} 1 & a \\ 1 & b \end{bmatrix}$$ and the determinant is $b-a \neq 0$. In the half-Neumann case you also have no problem; supposing the Neumann condition is on the left, you're looking at
$$\begin{bmatrix} 0 & 1 \\ 1 & b \end{bmatrix}$$
which is again invertible. But in the pure Neumann case you're looking at
$$\begin{bmatrix} 0 & 1 \\ 0 & 1 \end{bmatrix}$$
which is singular. This corresponds to the fact that $f(x)=c$ is a solution to the fully homogeneous problem (homogeneous ODE+ homogeneous BCs) for any $c$.
The situation changes with $y''=\lambda y$ with nonzero $\lambda$. In this case the pure Neumann matrix is $\begin{bmatrix} \sqrt{\lambda} e^{\sqrt{\lambda} a} & -\sqrt{\lambda} e^{-\sqrt{\lambda} a} \\ \sqrt{\lambda} e^{\sqrt{\lambda} b} & -\sqrt{\lambda} e^{-\sqrt{\lambda} b} \end{bmatrix}$ and the determinant is $\lambda(e^{\sqrt{\lambda}(b-a)}-e^{-\sqrt{\lambda}(b-a)})$. So the requirement now is is that $2\sqrt{\lambda}(b-a)$ isn't an integer multiple of $2\pi i$. If instead it is, then you have nontrivial homogeneous solutions given by cosines.
The general theory underlying this kind of question is called the Fredholm alternative, but it comes with some functional analysis baggage to understand, especially because we usually care about non-compact operators.