Garden lime can do it, but it adds ... calcium and something else? can't recall but the gauranteed analysis label has all of that info. So, just have to maake sure you don't overload the Ca and whatever else it adds to substrate.
That on top of continuing, i assume, to ph-balance anything you put into the soil will be more effective than 1 or the other alone. pH is a log scale from 7 ("zero"). Each whole number away is 10x more h30+ (7) depending on direction.
Runoff is not always super accurate as to what exists in the substrate. You've 'rinsed' out some of what was there and hopefully restored a better balance as far as what remains when you fertigate or irrigate. It's likely less acidic than what your runoff says. So, how does the plant look? Any issues? Then the pH is probably fine, because approaching 5.5 and below you encounter availability issues with Ca before other things.