Here are some hints:
What do you know about determinants and invertibility?
Alternatively, row reduce the matrix. Since you've already noted that $a = 0$ makes the matrix invertible, you needn't worry about this case when row reducing.
For row reduction, I'll do the first step so you can see how it's done. Let's have $R_2 \rightarrow R_1-aR_2$ (i.e. in place of row 2 put row 1 - $a$ times row 2). Then the matrix becomes
$$\left(\begin{array}{c} a & 1 & 1 \\ 0 & 1-a^2 & 1-a \\ 1 & 1 & a\end{array}\right).$$
Doing the same thing for row 3 (that is row 3 goes to row 1 minus $a$ times row 3) gives
$$\left(\begin{array}{c} a & 1 & 1 \\ 0 & 1-a^2 & 1-a \\ 0 & 1-a & 1-a^2\end{array}\right).$$
We want to eliminate downwards again. Before doing so, note that if $a=1$, our second row becomes $0$, meaning that for $a=1$, our matrix is not invertible (since it is row equivalent to a matrix with a row of zeroes). With that said, let's replace row 3 by row 3 times $1+a$ minus row 2. Then our matrix becomes
$$\left(\begin{array}{c} a & 1 & 1 \\ 0 & 1-a^2 & 1-a \\ 0 & 0 & 1+a-a^2-a^3-1+a\end{array}\right).$$
The lower right element can be rewritten as $2a - a^2 -a^3.$ For our matrix to not be invertible, we need this element to be $0$ (so we have a row of zeroes). But the zeroes of this are $a = 0,1,-2$. We've already ruled out $a=0$ as a solution (well you did that) and accounted for $a=1$ as a value that makes the matrix noninvertible so the only other solution is $a=-2$.
So for $a=1,-2$ the matrix is not invertible.