There is an error in your attempts when you write, e.g.
$$
\quad \quad\gcd(2a-b,4a)
\\ \to \quad \{a:4a\nmid2a-b\}
$$
because it is possible that $\gcd(2a-b,4a)$ is greater than $1$, so that the fraction reduces, even while simultaneously we do not have such a strong statement as $4a$ dividing $2a - b$. (e.g. $2a-b$ is even but not divisible by $4$ or by $a$.)
Instead, here's a useful fact:
$$
\gcd(xy,z) = 1 \quad\iff\quad \gcd(x,z) = 1 \text{ and } \gcd(y,z) = 1
$$
Therefore, we have that
\begin{align*}
\gcd(2a-b,4a) = 1
&\iff \gcd(2a-b,4) = 1 \text{ and } \gcd(2a-b,a) = 1 \\
&\iff b \text{ is odd,} \text{ and } \gcd(a,b) = 1. \\
\end{align*}
This gives you the condition you want: $a,b$ relatively prime and $b$ odd.