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this article, the authors provide a solution to the long-standing problem of understanding natural operations on the Hochschild cochain complex. For this, they organize such operations into a dg operad \\(\\mathcal{B}\\) which turns out to have the homotopy type of the little \\(2\\)-disks operad with inverted grading \\(C_{-*}D_2\\).NEWLINENEWLINEMore precisely, they construct an \\(\\mathbb{N}\\)-colored operad \\(B=\\{B^l_{k_1,...,k_n}\\}\\), where each \\(B^l_{k_1,...,k_n}\\) consists of trees giving rise to operations of the form \\(C^{k_1}(A,A)\\otimes ...\\otimes C^{k_n}(A,A)\\rightarrow C^l(A,A)\\) on the Hochschild cochain complex \\(C^*(A,A)\\) of an associative algebra \\(A\\) (the natural operations). They first compare these natural operations with a more categorical notion of natural operation, which acts on the endomorphism operad of any monoid in any symmetric monoidal category. Such operations form another \\(\\mathbb{N}\\)-colored operad which turns out to be isomorphic to \\(B\\) (Theorem A), thus the two notions of natural operation are equivalent.NEWLINENEWLINETo the \\(\\mathbb{N}\\)-colored operad \\(B\\) they associate a family of functors \\(\\{B_{\\bullet_1,...,\\bullet_n}^{\\bullet}:\\Delta\\times(\\Delta^{\\mathrm{op}})^n\\rightarrow \\mathrm{Ab}\\}_{n\\in\\mathbb{N}}\\), then they apply the multisimplicial totalization and cosimplicial totalization to get the dg operad \\(\\mathcal{B}\\) of natural operations. The second main theorem of this article (Theorem B) asserts that \\(\\mathcal{B}\\) has the homotopy type of \\(C_{-*}D_2\\). This actually follows from the more general Theorem C, proving that several suboperads of \\(\\mathcal{B}\\) have the homotopy type of \\(C_{-*}D_2\\), including \\(\\mathcal{B}\\) itself and the operad of braces. The case of natural operations on non-unital algebras is addressed as well.NEWLINENEWLINEThe crux of this work is the notion of crossed interval group which consists roughly of a sequence of groups \\(H=\\{H_n\\}\\) and an associated category \\(\\mathcal{I}H\\) giving rise to an adjunction \\(F_H:\\mathcal{C}^{\\Delta}\\leftrightarrows \\mathcal{C}^{\\mathcal{I}H^{\\mathrm{op}}}:U\\), where \\(\\mathcal{C}\\) is a cocomplete category and \\(\\mathcal{C}^{\\Delta}\\) the category of cosimplicial objects in \\(\\mathcal{C}\\). The functor \\(U\\) is the forgetful functor and \\(F_H\\) is a ``crossed interval extension''. In the particular case where \\(\\mathcal{C}\\) is the category of chain complexes, the cosimplicial totalization of the unit of this adjunction is a homotopy equivalence (Theorem 4.4). The authors show that the dg operad \\(\\mathcal{B}\\) is the cosimplicial totalization of a certain crossed interval extension, which is, using the aforementioned result, homotopy equivalent to a dg operad already well known by an earlier work of \\textit{M. A. Batanin} and \\textit{C. Berger} [Contemp. Math. 504, 23--52 (2009; Zbl 1221.18006)]. 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