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Let  \\[  (Au)(x) = -\\sum_{j,k=1}^n\\partial_j(a_{jk}(x)\\partial_k u)(x) + a(x)u(x)  \\]  be symmetric and uniformly strongly elliptic in \\({\\mathbb R}^n\\) with real \\(C_b^{\\infty}\\) coefficients. The authors consider realizations of \\(A\\) in \\(L^2({\\mathbb R}^n)\\) subject to coupling conditions of \\(\\delta\\)- and \\(\\delta'\\)-type supported on \\(\\Sigma\\). More precisely, let \\(A_{\\delta,\\alpha}\\) be the operator that acts like \\(A\\) on functions \\(u_{\\pm} \\in H^2(\\Omega_{\\pm})\\) such that \\(u_+\\big|_{\\Sigma} = u_-\\big|_{\\Sigma}\\) and \\(\\nu^+u_+ + \\nu^-u_- = \\alpha u\\big|_{\\Sigma}\\), where \\(\\nu^{\\pm}u_{\\pm}\\) are the outward conormal derivatives on \\(\\Sigma\\) of \\(u_{\\pm}\\) from the respective sides, and \\(\\alpha \\in C^{\\infty}(\\Sigma)\\) is real-valued. Similarly, \\(A_{\\delta',\\beta}\\) is the operator that acts like \\(A\\) on functions \\(u_{\\pm} \\in H^2(\\Omega_{\\pm})\\) such that \\(\\nu^+u_+ + \\nu^-u_- = 0\\) on \\(\\Sigma\\), and \\(u_+\\big|_{\\Sigma} - u_-\\big|_{\\Sigma} = \\beta \\nu^+u_+\\) with a real-valued function \\(\\beta \\in C^{\\infty}(\\Sigma)\\) that is nowhere vanishing. These realizations of \\(A\\) in \\(L^2({\\mathbb R}^n)\\) are self-adjoint and bounded from below. Let \\(A_0\\) denote the free realization of \\(A\\) in \\(L^2({\\mathbb R}^n)\\) with domain \\(H^2({\\mathbb R}^n)\\). Assuming invertibility of all operators (which can be obtained after shifting), the authors consider the resolvent differences \\(A_{\\delta,\\alpha}^{-1} - A_0^{-1}\\) and \\(A_{\\delta',\\beta}^{-1} - A_0^{-1}\\) in \\(L^2({\\mathbb R}^n)\\). These are compact operators, and the authors prove asymptotic formulas for their singular values. More precisely, they show that  \\[  s_k(A_{\\delta,\\alpha}^{-1} - A_0^{-1}) = C_{\\delta,\\alpha}k^{-\\frac{3}{n-1}} + o(k^{-\\frac{3}{n-1}})  \\]  as \\(k \\to \\infty\\), where the remainder improves to \\(O(k^{-\\frac{4}{n-1}})\\) if \\(\\alpha\\) is nowhere vanishing on \\(\\Sigma\\), and  \\[  s_k(A_{\\delta',\\beta}^{-1} - A_0^{-1}) = C_{\\delta'}k^{-\\frac{2}{n-1}} + O(k^{-\\frac{3}{n-1}})  \\]  as \\(k \\to \\infty\\). The authors give explicit formulas for the leading constants \\(C_{\\delta,\\alpha}\\) and \\(C_{\\delta'}\\) (where \\(C_{\\delta'}\\) is independent of \\(\\beta\\)). They also prove a similar asymptotic formula for the singular values of the resolvent difference of the \\(\\delta'\\)-realization and the two-sided Neumann realization instead of the free realization.  The proof is based on pseudodifferential techniques for boundary value problems (Boutet de Monvel's calculus) and Krein-type resolvent formulas which reduce the problem to classical results on spectral asymptotics of pseudodifferential operators on closed manifolds (here applied to operators on 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