Let be a metric space with doubling measure and a one-to-one operator of type having a bounded -functional calculus in satisfying the reinforced off-diagonal estimates on balls, where and . Let be a function such that is an Orlicz function, $\varphi(\cdot,t)\in {\mathbb A}{\infty}()$ (the class of uniformly Muckenhoupt weights), its uniformly critical upper type index and satisfies the uniformly reverse H"older inequality of order . In this paper, the authors introduce a Musielak-Orlicz-Hardy space , via the Lusin-area function associated with , and establish its molecular characterization. In particular, when is nonnegative self-adjoint and satisfies the Davies-Gaffney estimates, the atomic characterization of is also obtained. Furthermore, a sufficient condition for the equivalence between and the classical Musielak-Orlicz-Hardy space is given. Moreover, for the Musielak-Orlicz-Hardy space associated with the second order elliptic operator in divergence form on or the Schr"odinger operator with $0\le V\in L^1{}(^n)$, the authors further obtain its several equivalent characterizations in terms of various non-tangential and radial maximal functions; finally, the authors discuss the boundedness of the Riesz transform .

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