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The best effect for a splitter would possibly be Explosive because it deals explosive damage to an area and not only a single target. Think of the Spray'n'Pray, which has got it for example.
I do not believe Irradiated to give Nuclear Material, but rather Plasma Infused. I use Irradiated all the time and have not seen any Nuclear Material in the loot.
I'd go with Wounding.
That being said the extra plasma damage is defintely a good one.
Unlimited ammo is another good one never having to reload basically a pump action plasma shotgun.
The armor penetration is super underrated if you wanna got for enemies like mirlurks.
Also some legendary mods are applied to each projectile and weapons with more than one projectile per shot have better benefits from this.
Thus my opinion is "Freezing" and "Wounding". ("Plasma infused" - ballistic only)
Maybe "Two Shot" and "Furious"(*) will have a good outcome too.
*Furious marked in the wiki as a melee/unarmed only mod, though in the game at least one kind of ranged ballistic weapon has its legendary instances.
Preset items like Splattercannon and The Problem Solver (both for Furious) can have whatever combination the developer decided to give them.
The crit part of freezing does apply to each pellet, but there is nothing to suggest that it stacks on a single target so it only matters if you crit multiple targets at once. You are only likely to see this under the influence of Overdrive.
Two Shot on shotguns adds so much to their spread that they become almost unusable at any range outside of the targets nostrils, I would expect this to be the same for splitter guns, if plasma can even spawn with two shot.