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However, the limitation of Gaussian random variables on its computational complexity or sparsity affects the efficiency and accuracy. This paper proposes a novel approach for the optimization of measurement matrix in compressive sensing (CS) theory for hyperspectral unmixing. Firstly, a new Toeplitz-structured chaotic measurement matrix (TSCMM) is formed by pseudo-random chaotic elements, which can be implemented by a simple hardware; secondly, rank revealing QR factorization with eigenvalue decomposition is presented to speed up the measurement time; finally, orthogonal gradient descent method for measurement matrix optimization is used to achieve optimal incoherence. 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