Bex was kind enough to check up on this with the proper people in the dev team.

The official word on Barrage mechanics:

"Barrage spends the first 40% of the attack time doing the wind up, and then
spends the remaining 60% firing the projectiles (each projectile takes a time t
hat is 60% of the attack time, divided by the number of projectiles, so regardle
ss of the number of projectiles, they take 60% of the attack time in total). The
attack thus takes the full attack time, regardless of number of projectiles."
It was literally that easy. Now, many of us got results that disprove the above,
however, in a previous statement from GGG (sorry, can't find it, help appreciat
ed), we do know that what happens between the client and the server is mismatche
d a bit (disclaimer: statement was made BEFORE net framework changes.) This migh
t account for the (previously?) mismatching when firing from a single position f
or a longer period of time.
Regardless, the breakpoints using the above data are as follows:
((1/A)*0.6) / P = Time between projectiles
A: Attacks per Second
P: Projectiles Fired
Note: 1/A = T, where T is your displayed Attack Time
(I just like to avoid possible rounding error)
Bold denotes "perfect" timing where each projectile lands just after the Cast on
Critical Strike internal timer (0.05s) resets (on a stationary target.)
Edit: (A quick note) So, you ask, why go any faster? The answer is, if you miss
a proc, repeated attacks within a single proc time frame (0.05s) decrease the ch
ances that you'll go an entire proc period without a spell cast. This, in turn,
makes it more likely to cast more spells on average.
Barrage (4 Projectiles):
<1.5 APS
<3
<4.5
etc.
Barrage + Enchantment (5 Projectiles):
<1.2 APS
<2.4
<4.8
Barrage + LMP (6 Projectiles):Whyareyoudoingthis...
<2 APS
<4
Barrage + LMP + Enchantment (7 Projectiles):Thisisstillweird...
<1.71429 APS
<3.42857
Barrage + GMP (8 Projectiles):
<1.5 APS
<3 <4.5

Barrage + GMP + Enchantment (9 Projectiles):

<1.333 APS
<2.667
<5.333
Now you can play with your CoC properly. (#Deadhorse)