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The main results are concerned with free ergodic probability-measure-preserving (pmp) actions \\(\\Gamma \\curvearrowright (X,\\mu)\\) of \\textit{weakly amenable} groups \\(\\Gamma\\) on probability spaces \\((X,\\mu)\\). One problem of major interest concerns the uniqueness of the Cartan subalgebra \\(L^\\infty(X)\\) in the group measure space algebra \\(L^\\infty (X) \\rtimes \\Gamma\\). One important result that applies to a broad class of infinite discrete groups states that if, in addition, \\(\\Gamma\\) admits a proper \\(1\\)-cocycle into a non-amenable representation, or if (for instance) it has non-zero first \\(\\ell^2\\)-Betti number, then \\(L^\\infty(X)\\) is the unique Cartan subalgebra in \\(L^\\infty(X)\\rtimes \\Gamma\\) up to unitary conjugacy.  To illustrate the strength of this unique Cartan decomposition result, suppose that \\({\\mathbb F}_m \\curvearrowright (X,\\mu)\\) and \\({\\mathbb F}_n \\curvearrowright (Y,\\eta)\\) are two free ergodic pmp actions of the free groups \\({\\mathbb F}_m\\) and \\({\\mathbb F}_n\\) on \\(m\\) and respectively \\(n\\) generators. Combining the above result with a result of \\textit{D. Gaboriau} [Publ. Math., Inst. Hautes \u00c9tud. Sci. 95, 93--150 (2002; Zbl 1022.37002)], one concludes that if \\(L^\\infty (X)\\rtimes {\\mathbb F}_m \\cong L^\\infty (Y) \\rtimes {\\mathbb F}_n\\), then \\(m=n\\). Important applications concerning wreath product groups and treeable ergodic pmp equivalence relations are also given. For instance, it is shown that if the group von Neumann algebras defined by the groups \\({\\mathbb Z}^{({\\mathbb F}_m)} \\rtimes {\\mathbb F}_m\\) and \\({\\mathbb Z}^{({\\mathbb F}_n)} \\rtimes {\\mathbb F}_n\\) are isomorphic, then \\(m=n\\). It is also proved that if \\(L{\\mathcal R}_1 \\cong L{\\mathcal R}_2\\) for two treeable countable ergodic pmp equivalence relations \\({\\mathcal R}_1\\) and \\({\\mathcal R}_2\\), then \\({\\mathcal R}_1 \\cong {\\mathcal R}_2\\).  A relative strong solidity type dichotomy is established for a large class of weakly amenable groups \\(\\Gamma\\): an amenable subalgebra \\(A\\) of an arbitrary crossed product \\(B\\rtimes \\Gamma\\), with \\(B\\) amenable, either embeds into \\(B\\) in Popa's sense of ``intertwining-by-bimodules'' or it has amenable normalizer. This extends ground-breaking work of \\textit{N. Ozawa} [Acta Math. 192, No. 1, 111--117 (2004; Zbl 1072.46040)], \\textit{N. Ozawa} and \\textit{S. Popa} [Ann. Math. (2) 172, No. 1, 713--749 (2010; Zbl 1201.46054)], and \\textit{I. Chifan} and \\textit{T. Sinclair} [Ann. Sci. \u00c9c. Norm. Sup\u00e9r. (4) 46, No. 1, 1--33 (2013; Zbl 1290.46053)] on hyperbolic groups, and solidity and strong solidity in von Neumann algebras.  Another application of unique Cartan decomposition establishes \\(W^*\\)-superrigidity of quotients of the generalized Bernoulli action \\(\\Gamma_1 \\times \\Gamma_2 \\curvearrowright [0,1]^{\\Gamma_1 \\times \\Gamma_2}\\), where \\(\\Gamma_1\\) and \\(\\Gamma_2\\) are weakly amenable icc groups that admit a proper \\(1\\)-cocycle into a non-amenable representation. Finally, it is proved that if \\(\\Gamma\\) and \\(\\Lambda\\) are icc groups that satisfy the requirements from the main unique Cartan decomposition theorem, and act outerly on the hyperfinite II\\(_1\\) factor \\(R\\) and such that \\(R\\rtimes \\Gamma \\cong R\\rtimes \\Lambda\\), then \\(\\Gamma \\cong \\Lambda\\) and the actions of \\(\\Gamma\\) and \\(\\Lambda\\) on \\(R\\) are cocycle 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