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It ends up that, assuming you're running a crit-focused build and not a pure strength build, the optimal ratio of improved damage and crit from souls is essentially exactly 50% each, if damage is your goal. This is true even if you have all 4 Serpent syllables and your "improved crit" is 3 times as strong, though that does make "Improve Crit" initially stronger for the first 3 minute (or first hour if not using Wind King).
For example, with around 10-15 souls, here's the overall multipliers after 15 minutes (or 5 hours without Wind King).
Only Damage or Crit: x6.97
50/50 Dmg & Crit: x15.88
Full Dmg & Crit (2 Souls) : x48.58
Only Serpent Crit: x18.91
50/50 Dmg & Serp Crit : x39.67
75/25 Serp Crit & Damage: x35.97*
Full Dmg & Serp Crit (2 Souls): x131.79
Here's the overall multipliers after 60 minutes (or 20 hours without Wind King...)
Only Damage or Crit: x24.88
50/50 Dmg & Crit: x167.43
Full Dmg & Crit (2 Souls) : x618.95
Only Serpent Crit: x72.64
50/50 Dmg & Serp Crit : x476.41
75/25 Serp Crit & Damage: x381.43*
Full Dmg & Serp Crit (2 Souls): x1,807.11
* Note that Serpent Crit starts off individually stronger than a split between damage and crit, however the longer it runs, the stronger a 50/50 split becomes relative to Serp Crit individually, or in other proportions.
As rob_s_cat2 mentioned, running primarily Improved Damage can potentially keep you from slowing down to crit things, but honestly if you're running a crit build your crits are probably going to be hundreds, if not thousands, of times stronger than your normal hits. If you're investing enough resources for your base damage to one-shot things, you're probably be better off running a build less focused on crits.
P.S. The secondary takeaway here is that Wind King Mask is very, very strong for progression (killing bosses). For a single skill point, you can have a x167 multiplier from souls after an hour, compared to x2.55 without Wind King. On the actual boss, turn on the Poison soul syllable from Serpent, which averages an additional x27.5 multiplier over a 3 minute period with Wind King (x2.35 without Wind King) for a total bonus multiplier of x4,592 and bosses melt very quick.