No. If magnesium is low, you will (may) be unable to maintain even normal levels of both calcium and alkalinity.
Under any circumstance (such as OK magnesium) if either calcium is too high or alkalinity is too high, the other will (may) be undesirably low.
Think of it this way: multiplying calcium times alkalinity cannot exceed a certain value. If both are normal, that's OK. If one is high, the other must be low, and vice versa.
In your case, alkalinity is too high, and that's why you can't boost calcium easily.