Here are some ideas and observations, not a complete answer.
It looks like a nonlinear regression problem to me,
but I would be curious about the nature of the model and its constraints,
whether any additional assumptions could be made,
and whether someone better qualified would have a look at this.
Let $a=(a_1~\cdots~~a_N)^T\in\mathbb{R}^{N\times1}$,
$1\equiv1_{N\times1}\in\mathbb{R}^{N\times1}$, and note that
$$
\left(
a(1-a)^T
\right)^T
=(1-a)a^T,
$$
so that $k_2$ and $k_3$ are coefficients of transposed matrices,
$$a(1-a)^T=a\cdot1_{1\times N}-aa^T$$
and
$$(1-a)a^T=1\cdot a^T-aa^T.$$
Let $A=k_1-k_2-k_3$, $B=k_2$ and $C=k_3$,
define the residual error matrix
$$
\begin{eqnarray}
E &=& k_1aa^T+k_2a(1-a)^T+k_3(1-a)a^T - T \\
&=& A\;aa^T+B\;a\cdot 1^T+C\;1\cdot a^T-T
\end{eqnarray}
$$
so that
$$
E_{ij} = A\;a_ia_j+B\;a_i+C\;a_j-T_{ij}.
$$
Now we want $E\approx0$. Does this look like a (nonlinear least squares) regression problem to anyone?
Notice that $A=C=0\ne B$ would model dependence of $T_{ij}$
on $i$ (equal rows $Ba_i=\frac1N\sum_jT_{ij}$),
that $A=B=0\ne C$ would model dependence on $j$
(equal columns $Ca_j=\frac1N\sum_iT_{ij}$),
and that a dominant $A$ models a (symmetric) covariance matrix.
Another ideal case would be when we could write
$$Aa_ia_j+Ba_i+Ca_j=(B_1a_i+B_0)(C_1a_j+C_0)-B_0C_0.$$
How could we exploit such a factorization,
and what condition would $T$ need to satisfy
(perhaps $NB_0C_0=\sum_{ij}T_{ij}$)?
Two (or three) possible target functions (to minimize) come to mind:
$EE^T$, $E^TE$ and $||E||^2$. (The first two are not identical unless $T=T^T$. Unfortunately we don't know that $T$ is symmetric,
and the whole point of having distinct $B$ & $C$ must be to allow
for nonsymmetric $T$, so it would probably be of no use to
take $\frac{T+T^T}{2}$ in place of $T$ above.)
If we take $||E||^2=\sum_{ij}E_{ij}^2$ as our target function,
then minimizing it boils down to solving the equations
$$
0=\frac12\frac{\partial}{\partial a_k}||E||^2
=\frac12\frac{\partial}{\partial a_k}\sum_{ij}
\left(A\;a_ia_j+B\;a_i+C\;a_j-T_{ij}\right)^2
$$
$$
=(2C^2)a_k^3
+3C(A+B)a_k^2
+\left[(A+B)^2-2CT_{kk}+\sum_{i\ne k}(A+Ca_i)^2+(B+Ca_i)^2\right]a_k
$$
$$
+\left[-(A+B)T_{kk}
+\sum_{i\ne k}
(A+Ca_i)(Ba_i-T_{ki})+
(B+Ca_i)(Aa_i-T_{ik})
\right]
$$
(or something similar, if I have made an error)
which involves cubic degree and interdependence,
and so does not look very tractable.
One could use the standard tricks involving average values of (rows/columns of) $T$ to get a little further, and use Gröbner Bases to find a solution
(if one exists). Or, one could avoid this
and use in stead the standard iterative approach
for nonlinear least squares regression.