Dipolar charge distributions are essentially all the same: regardless of how one adds up a combination of the form $$ \sigma(\theta,\varphi) = \operatorname{Re}\left[\sum_{m=-1}^1 a_m Y_{1m}(\theta,\varphi)\right], $$ you only ever get a rotated version of the canonical $Y_{10}(\theta,\varphi) \propto \cos(\theta)$, multiplied by some global constant.
Quadrupolar charge distributions, on the other hand, are more interesting, because you can have 'double peanut' distributions of the form $$ \sigma(\theta,\varphi) = \sin(\theta)\cos(\varphi)\cos(\theta) = \frac{xz}{r^2}, $$ but you can also have the usual two-balls-and-a-ring distribution of the form $$ \sigma(\theta,\varphi) = 3\cos^2(\theta)-1 = \frac{2z^2-x^2-y^2}{r^2}, $$ and those two are not rotations of each other. With that in mind, then:
If you consider two charge distributions to be equivalent if they differ only by a rigid rotation or by a global constant, how many real parameters do you need to describe quadrupolar charge distributions on the unit sphere of the form $$\sigma(\theta,\varphi) = \operatorname{Re}\left[\sum_{m=-2}^2 a_m Y_{2m}(\theta,\varphi)\right]?$$ What is the dimensionality of this manifold, and what is its topology? Can this reduction be done in a systematic way? And, if so, how? What is the physical significance of those parameters, and do they have set names in the literature?
Similarly, how do those questions look like for octupoles?
What about for general multipoles?
Edit: I guess, upon further reflection, what I'm asking for is the essential topology of the orbit space of the action of $\mathrm{SO}(3)$ on its irreducible representations: is the quotient space a manifold? if so, what are its dimensions and its topology? if not, why not? I would like to see this for arbitrary $\ell$ but with a specific emphasis on both $\ell=2$ and $\ell=3$, which strike me as the first two nontrivial examples. (I don't anticipate $\ell=4$ to be much more complicated than the octupole representation, but I do think that the octupole brings in nontrivial wrinkles compared to the quadrupole.) If people can comment on what happens for half-integral $j$ that would be awesome as well.
I am aware, in particular, of the reduction of the quadrupole representation by diagonalizing its coefficient matrix, but it is not at all clear to me how one would generalize this to the octupole layer's rank-3 tensors and beyond, and I would definitely like answers to address this generalization.
On the other hand, I do want the discussion to also address the particulars of these orbit spaces: what do the different points represent, and how do those charge distributions actually look like, at least at the 'extremal' points (like $Y_{20}$ and $\operatorname{Re}(Y_{22})$). The dimension-counting argument in Logan's answer is interesting, but it indicates that there are $2\ell-2$ non-equivalent distributions at $\ell\geq 2$, and this means that several of those dimensions are not encompassed by the usual spherical harmonics: since $\operatorname{Re}(Y_{\ell ,\pm m})$ and $\operatorname{Im}(Y_{\ell ,\pm m})$ are rotation-equivalent, when taken neat the $Y_{\ell m}$ can only produce up to $\ell+1$ distinct distributions (with one knocked out at $\ell=2$ by rotational equivalence), this means that from $\ell=4$ onwards there need to be at least $\ell-3$ independent linear combinations of the $Y_{\ell m}$ that are not rotationally equivalent to any of them. What do these combinations look like? I would like explicit examples for the first nontrivial cases, as well as systematic methods to get them for arbitrary $\ell$.
Now, I realize that this whole package is a big ask, but I do think it's interesting and worth exploring. I'll probably add some fake-internet-points sweetener in a few days, but I do want more in-depth answers than the current ones.