As you suggest in your question, the moment generating function holds information on the moments of a distribution. Except for notable examples (e.g. Bernoulli random variable) where the first moment also coincides with the probability of success of the trial, to the best of my knowledge don't hold any direct information on the probability mass.
What you are probably interested in is the probability generating function of a distribution. This on the other hand contains information on the probability mass associated to each value of the random variable's spectrum.
For a discrete non-negative random variable $X$ with $x \in \mathbb{N}$ and probability mass function $p$, then the probability generating function of $X$ is defined as
$$G_X(z) = E(z^X) = \sum_{x=0}^\infty p(x)z^x$$
The logic of it is very similar to that of a moment generating function: a clothesline where instead of hanging moments we hang probabilities of points on the spectrum. Taking the appropriate derivative and evaluating the function at 0 we obtain
$$P(X=k) = \frac{d^{(k)}}{dt^k}\frac{G_X(0)}{k!}$$
---Edit---
I'm sorry, I did not read the question thoroughly enough the first time, I'll clarify better off now.
One way you could go by doing this is using the connection between the mgf and the pgf of a discrete random variable. Using your definition of moment generating function and my definition of probability generating function, we can say that
$$M_Y(t) = E(e^{tY}) = G_Y(e^t)$$
and so a way to obtain probabilities directly from the moment generating function could be the following
$$\frac{1}{k!}\frac{d^{(k)}}{dt^k}M_Y(log(t)) \quad \text{evaluated at} \quad t=0$$
In your example, we would have
$$M_Y(log(t)) = \frac{2^{log(t)} + e^{3log(t) + 4k}}{3}$$
If you wanted to find $P(X=1)$, you would take the first derivative and let $t=0$.