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In this paper we work out in detail a new proposal to define rigorously a sector of loop quantum gravity at the diffeomorphism invariant level corresponding to homogeneous and isotropic cosmologies, and propose how to compare in detail the physics of this sector with that of loop quantum cosmology. The key technical steps we have completed are (a) to formulate conditions for homogeneity and isotropy in a diffeomorphism covariant way on the classical phase space of general relativity, and (b) to translate these conditions consistently using well-understood techniques to loop quantum gravity. To impose the symmetry at the quantum level, on both the connection and its conjugate momentum, the method used necessarily has similiarities to the Gupta–Bleuler method of quantizing the electromagnetic field. Lastly, a strategy for embedding states of loop quantum cosmology into this new homogeneous isotropic sector, and using this embedding to compare the physics, is presented. [ABSTRACT FROM AUTHOR]