One can tackle this question by forming an offset grid of squares of radii $1/k$ in a roughly triangular fashion that fits inside the top left sector of the rectangle, whereby the squares can be filled with circles and we are done.
To formalize this idea, let us begin by giving ourselves enough leeway to only need the top left sector. The calculation in the post notes we don't need much of the remaining area if we fill in the first $n = 20$ balls, but to give ourselves way more room (and since we need it later anyway), let's instead fill in the first $65$ balls by hand so we can start with $n=66$:
![enter image description here](https://cdn.statically.io/img/i.sstatic.net/4hr0g.pngm.png)
(Desmos graph here, modified from the OP's graph)
Now that we have this, our goal will be to construct a triangle in the top left sector out of boxes, with radii as such:
![enter image description here](https://cdn.statically.io/img/i.sstatic.net/T99jcm.png)
There is, of course, the question of how to make the squares tangent when the radii are decreasing, so we stipulate that at each stage we first put a box as far left and then as far up as possible, and then put the remaining boxes flush against the top right of the associated box from the prior step. Graphically, where a box is labeled $m$ if it's added in the $m$th step, this looks like:
![enter image description here](https://cdn.statically.io/img/i.sstatic.net/lRtDdm.png)
If we draw a line with angle $45 \deg$ at the bottom right of the bottom-most box, we get a bounding box for a triangle:
![enter image description here](https://cdn.statically.io/img/i.sstatic.net/KpmYum.png)
The short side length of this isosceles triangle is given by first summing the diameters of the column of leftmost boxes and then adding the diameter of the bottom-left box. Specifically, if we realize the triangular numbers $T_n = \frac{n(n+1)}{2}$ are involved, we can bound the side length $S_m$ at the $m$th stage of the construction as:
$$S_m = \frac{2}{n + \frac{m(m-1)}{2}} + \sum_{k=0}^{m-1} \frac{2}{n + \frac{k(k+1)}{2}} \le \frac{2}{n} + \sum_{k=0}^{\infty} \frac{2}{n + \frac{k(k+1)}{2}}$$
Indeed, here we use the fact $n = 66$ to determine:
$$S_m \le \frac{2}{66} + \sum_{k=0}^{\infty} \frac{2}{66 + \frac{k(k+1)}{2}} = \frac{2}{66} + \frac{4\pi \tanh \left(\frac{\sqrt{527} \pi}{2} \right)}{\sqrt{527}} = 0.577703\ldots$$
Now, this is important, because it turns out to be a good enough bound. Indeed, if one draws the tangent line to the unit circle in the OP's diagram at the point $(\cos(3\pi/4), \sin(3\pi/4))$ and sees where it intersects the vertical boundary on the left, a quick calculation (using the fact the line has equation $y = x + \sqrt{2}$) shows the largest possible isosceles triangle which can fit has short side length $2 - \sqrt{2} = 0.585786\ldots$, so our triangle constructed above fits!
![enter image description here](https://cdn.statically.io/img/i.sstatic.net/2plwdm.png)
As a sanity check, we can now put the remaining circles of radius $1/k$ into the boxes of radius $1/k$ and determine the resulting area. Indeed, the area of the boxes can be calculated as $\sum_{k = 66}^\infty \left(\frac{2}{k}\right)^2 \approx 0.061$ while the area of the top-left sector is given by $1 - \frac{\pi}{4} \approx 0.21$, so we end up with plenty of area to spare.