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The rotation about the CoM is the (instantaneous) motion in the CoM instantaneous rest frame. The separation into CoM angular momentum and angular momentum due to the CoM motion is simply a convenient way of doing the bookkeeping of the angular momentum as the terms separate.
Consider a system of rigidly connected masses ##m_i## with positions ##\vec x_i## and velocities ##\vec v_i## relative to a fixed point of the rotation with angular velocity ##\vec \omega##. By assumption of the rigidity:
$$
\vec v_i = \vec\omega \times \vec x_i
$$
and so the total angular momentum relative to the fixed point is
$$
\vec L = \sum_i m_i \vec x_i \times (\vec \omega \times \vec x_i)
= \sum_i m_i [r_i^2 \vec \omega - (\vec\omega\cdot \vec x_i)\vec x_i]
$$
where ##r_i## is the magnitude of ##\vec x_i##. This is the usual expression involving what is essentially the definition of the moment of inertia relative to the fixed point.
We can now rewrite this by introducing a reference displacement ##\vec x_0## and the instantaneous rigid velocity ##\vec v_0 = \vec\omega \times \vec x_0## of that point. We introduce ##\vec x_i = \vec y_i + \vec x_0## and ##\vec v_i = \vec u_i + \vec v_0##, where ##\vec y_i## and ##\vec u_i## are the position and velocity of mass ##i## relative to the reference displacement and velocity.
The angular momentum about the fixed point now takes the form
$$
\vec L = \sum_i m_i (\vec y_i + \vec x_0)\times (\vec \omega \times \vec y_i + \vec v_0)
= \sum_i m_i[R_i^2 \vec \omega - (\vec y_i\cdot \vec\omega)\vec y_i]
+ M \vec x_0 \times \vec v_0
+ \sum_i m_i [\vec x_0 \times (\vec\omega \times \vec y_i) + \vec y_i \times \vec v_0]
$$
with ##R_i## the magnitude of ##\vec y_i## and ##M = \sum_i m_i## (ie, the total mass). The first term here is now the angular momentum of the system relative to the reference displacement in the instantaneous rest frame of the reference displacement. The second term is the angular momentum of a single particle of mass ##M## at the reference displacement relative to the original fixed point. The last term is quite messy.
However, if you take the CoM as the reference displacement, then ##\sum_i m_i \vec y_i = 0## by definition and the last two terms vanish. Voilà, you have reexpressed the total angular momentum relative to the fixed point as the angular momentum relative to the CoM (in the CoM instantaneous rest frame) plus the angular momentum of a point mass at the CoM moving at the CoM velocity.
The advantage over the first expression is that the moment of inertia relative to the CoM is often much easier to express in terms of standard moments of inertia that have already been computed. Many times simplifying computation.
Iirc, this is also covered in some detail in chapter 10 of my book.
Consider a system of rigidly connected masses ##m_i## with positions ##\vec x_i## and velocities ##\vec v_i## relative to a fixed point of the rotation with angular velocity ##\vec \omega##. By assumption of the rigidity:
$$
\vec v_i = \vec\omega \times \vec x_i
$$
and so the total angular momentum relative to the fixed point is
$$
\vec L = \sum_i m_i \vec x_i \times (\vec \omega \times \vec x_i)
= \sum_i m_i [r_i^2 \vec \omega - (\vec\omega\cdot \vec x_i)\vec x_i]
$$
where ##r_i## is the magnitude of ##\vec x_i##. This is the usual expression involving what is essentially the definition of the moment of inertia relative to the fixed point.
We can now rewrite this by introducing a reference displacement ##\vec x_0## and the instantaneous rigid velocity ##\vec v_0 = \vec\omega \times \vec x_0## of that point. We introduce ##\vec x_i = \vec y_i + \vec x_0## and ##\vec v_i = \vec u_i + \vec v_0##, where ##\vec y_i## and ##\vec u_i## are the position and velocity of mass ##i## relative to the reference displacement and velocity.
The angular momentum about the fixed point now takes the form
$$
\vec L = \sum_i m_i (\vec y_i + \vec x_0)\times (\vec \omega \times \vec y_i + \vec v_0)
= \sum_i m_i[R_i^2 \vec \omega - (\vec y_i\cdot \vec\omega)\vec y_i]
+ M \vec x_0 \times \vec v_0
+ \sum_i m_i [\vec x_0 \times (\vec\omega \times \vec y_i) + \vec y_i \times \vec v_0]
$$
with ##R_i## the magnitude of ##\vec y_i## and ##M = \sum_i m_i## (ie, the total mass). The first term here is now the angular momentum of the system relative to the reference displacement in the instantaneous rest frame of the reference displacement. The second term is the angular momentum of a single particle of mass ##M## at the reference displacement relative to the original fixed point. The last term is quite messy.
However, if you take the CoM as the reference displacement, then ##\sum_i m_i \vec y_i = 0## by definition and the last two terms vanish. Voilà, you have reexpressed the total angular momentum relative to the fixed point as the angular momentum relative to the CoM (in the CoM instantaneous rest frame) plus the angular momentum of a point mass at the CoM moving at the CoM velocity.
The advantage over the first expression is that the moment of inertia relative to the CoM is often much easier to express in terms of standard moments of inertia that have already been computed. Many times simplifying computation.
Iirc, this is also covered in some detail in chapter 10 of my book.