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The matrix inner product defined by \\(W\\) is  \\[ (P,Q)_W= \\int_{\\mathbb{R}} P(t) dW(t)Q^*(t)\\in M_{N\\times N}, \\]  with \\(P,Q\\in P_{N\\times N}\\), where \\(M_{N\\times N}\\) is the space of numerical \\(N\\times N\\) matrices, \\(P_{N\\times N}\\) is the space of \\(N\\times N\\) matrix polynomials and \\(Q^*\\) is the Hermitian adjoint of \\(Q\\).   The author characterizes the positive definite matrices of measures whose matrix inner product has a symmetric left-hand side matrix second-order differential operator of the form  \\[ \\ell_{2,L}= A_2D''+ A_1D'+ A_0 D^0. \\]  Next, the author establishes a relationship between the existence of a symmetric left- or right-hand side matrix second-order differential operator for the matrix inner product defined by \\(W\\). Then the author treats the existence of a second-order differential equation which satisfies a sequence of orthogonal matrix polynomials with respect to \\(W\\) and the existence of a recurrence formula for the moments of \\(W\\).   In the third part, the author proves a characterization theorem by reducing the problem to the scalar case, and shows that the positive definite matrix of measures exists, for which a symmetric left-hand side second-order differential operator exists.   In the last part, the author shows a counterexample which proves that the classification theorem does not work for right-hand side second-order differential 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