We extend and deepen the theory of functional calculus for semigroup generators, based on the algebra $\mathcal B$ of analytic Besov functions, which we initiated in a previous paper. In particular, we show that our construction of the calculus is optimal in several natural senses. Moreover, we clarify the structure of $\mathcal B$ and identify several important subspaces in practical terms. This leads to new spectral mapping theorems for operator semigroups and to wide generalisations of a number of basic results from semigroup theory.
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