From what I understand, which isn't much, you would probably want to increase the minerals (Ca + SO4) for the entirety of the batch (not just mashing) because this does a lot more than just increase efficiency.
Quote:
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Originally Posted by HowToBrew
Ca
Calcium is the principal ion that determines water hardness and has a +2 charge. As it is in our own bodies, calcium is instrumental to many yeast, enzyme, and protein reactions, both in the mash and in the boil. It promotes clarity, flavor, and stability in the finished beer. Calcium additions may be necessary to assure sufficient enzyme activity for some mashes in water that is low in calcium.
SO4
Brewing Range = 50-150 ppm for normally bitter beers, 150-350 ppm for very bitter beers
The sulfate ion also combines with Ca and Mg to contribute to permanent hardness. It accentuates hop bitterness, making the bitterness seem drier, more crisp.
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I would say pH is less of a factor unless you are getting horrible efficiency even when using 5.2pH.
I am far from an expert on water chemistry, I only know what I have read from HowToBrew and haven't enacted any of these methods yet. I hope someone with more experience stops in and can offer some more advice.