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2-Arsa-1,3-butadienes (L)As(cAACR) (L = PhC[double bond, length as m-dash]C(NDipp)CH2, Dipp = 2,6-iPr2C6H3; cAACR = C(NDipp)CMe2CH2C(R), R = Me2 2a, R = cyclohexyl (Cy) 2b) and the corresponding radical cations [(L)As(cAACR)]GaCl4 (R = Me2 3a, Cy 3b) and dications [(L)As(cAACR)](GaCl4)2 (R = Me 4a, Cy 4b) featuring a C[double bond, length as m-dash]C-As[double bond, length as m-dash]C π-conjugated framework are reported.We have developed a novel near-infrared ratiometric fluorescent theranostic nanoprobe. Upon reaction with glutathione, it