Find $~k ~: \arg[ ~(k - 4) + i(5k + 1) ~] = 2\pi/3.$
This answer is much more longwinded than it would be if I employed the tangent function. However, from "An Introduction To Complex Function Theory" (Bruce Palka) - Chapter 1, I have learned a method that uses the sine and cosine functions, and avoids any confusion.
The ironclad rule is:
Given $~z = x + iy \neq 0 + i0.$
Compute $~\displaystyle r = \sqrt{x^2 + y^2} \implies r > 0.$
Compute $~\theta~$ as the unique angle, within a modulus of $~2\pi,~$
such that $~\displaystyle \cos(\theta) = \frac{x}{r}, ~\sin(\theta) = \frac{y}{r}.$
Note that by the definition of $~r,~$ this implies that
$\cos^2(\theta) + \sin^2(\theta) = 1.$
A common convention, which I will follow in this answer, is to set $~\theta~$ as the unique satisfying angle, in the range $~-\pi < \theta \leq \pi.~$
So, all of the above groundwork will serve as the basis for attacking the problem.
Here, you are given that the corresponding angle, that represents $~z = x + iy~$ is $~2\pi/3.$
This implies that $~\displaystyle \cos(\theta) = \frac{-1}{2}, ~\sin(\theta) = \frac{\sqrt{3}}{2}.$
By the premise, you have that
$x = k - 4.$
$y = 5k + 1.$
This implies that
$$r = \sqrt{(k-4)^2 + (5k+1)^2}$$
$$= \sqrt{(k^2 - 8k + 16) + (25k^2 + 10k + 1)}$$
$$= \sqrt{26k^2 + 2k + 17}.$$
Therefore,
$$\frac{-1}{2} = \frac{k-4}{\sqrt{26k^2 + 2k + 17}} \tag1 $$
and
$$\frac{\sqrt{3}}{2} = \frac{5k+1}{\sqrt{26k^2 + 2k + 17}}. \tag2 $$
At this point, the goal is to find all values of $~k~$ (if any) that satisfy both (1) and (2) above. Any such satisfying value of $~k~$ must be construed to be a satisfying answer.
To facilitate the computations, I will compute $~\cos^2(\theta)~$ and $~\sin^2(\theta),~$ based on (1) and (2) above. This will identify all possible candidate values of $~k,~$ (if any). Then, each candidate value will have to be individually scrutinized to see if it satisfies both (1) and (2) above.
So,
$$\frac{1}{4} = \frac{k^2 - 8k + 16}{26k^2 + 2k + 17} \tag3 $$
and
$$\frac{3}{4} = \frac{25k^2 + 10k + 1}{26k^2 + 2k + 17}. \tag4 $$
The easiest way to proceed is to recognize that while (3) and (4) share the same RHS denominator, you must have the RHS numerator of (3) is $~1/3~$ of the RHS numerator of (4).
Therefore,
$$3 \times (k^2 - 8k + 16) = (25k^2 + 10k + 1) \implies $$
$$3k^2 - 24k + 48 = 25k^2 + 10k + 1 \implies $$
$$22k^2 + 34k - 47 = 0 \implies $$
$$k = \frac{1}{44} \left[ ~-34 \pm \sqrt{1156 + 4136} ~\right] $$
$$= \frac{1}{44} \left[ ~-34 \pm \sqrt{5292} ~\right] $$
$$= \frac{1}{44} \left[ ~-34 \pm \sqrt{(42)^2 \times 3} ~\right]$$
$$= \frac{1}{44} \left[ ~-34 \pm 42\sqrt{3} ~\right]. \tag5 $$
So, the two values in (5) above represent the candidate values for $~k.$
From (1) above, you must have that $~k - 4 < 0,~$ and from (2) above, you must have that $~(5k+1) > 0.$
So, you must have that $~-1/5 < k < 4.~$
Note that $~\displaystyle 42\sqrt{3} \approx 72.75,~$ so you can immediately reject the candidate value of
$$\frac{1}{44} \left[ ~-34 - 42\sqrt{3} ~\right].$$
Further, the candidate value of
$$\frac{1}{44} \left[ ~-34 + 42\sqrt{3} ~\right] \approx \frac{38.75}{44}, \tag6 $$
so this candidate value is in range.
It only remains to verify that the candidate value of $~k~$ in (6) above does in fact satisfy the original constraints represented by (1) and (2). By collectively examining the constraints represented by (1), (2), (3), and (4), walking through the computations that followed (3) and (4), and noting that
$$(k-4)^2 + (5k+1)^2 = 26k^2 + 2k + 17,$$
you can deduce that the candidate value of $~k~$ in (6) above does satisfy the original constraints in (1) and (2).
$\underline{\text{Addendum}}$
This addendum is beyond the scope of the original problem, which may be regarded as
"analytical geometry meets complex analysis", and so this addendum may well initially confuse the original poster.
In analytical geometry, the domain of the sine and cosine functions are angles, while in real analysis (AKA calculus), the domain of the sine and cosine functions are arc lengths of the unit circle (i.e. circle of radius 1).
Normally, complex analysis is considered an extension of real analysis, so normally, in complex analysis, the domain of the sine and cosine functions are arc lengths of the unit circle.
However, this specific problem is somewhat unusual in that it actually represents
"analytical geometry meets complex analysis".
That is, none of the real analysis extensions into complex analysis are relevant here. For example, this problem does not involve any differentiation, integration, or taylor series.
So, in this somewhat unusual problem, the domain of the sine and cosine functions may (harmlessly, and for the sake of simplicity) be regarded as angles.
Here, the unit circle arc length of $~2\pi/3~$ is represented by the angle $~120^\circ.$
See also this answer for a discussion of the term radian in real analysis.