We disclose the intrinsic semiconducting properties of one of the largest mixed-valent uranium clusters, [Single-crystal X-ray crystallography demonstrates that U V center is stabilized within a tetraoxo core surrounded by eight uranyl(VI) pentagonal bipyramidal centers. The oxidation states of uranium are substantiated by spectroscopic data and magnetic susceptibility measurement. Electronic spectroscopy and theory corroborate that U V species serve as electron donors and thus facilitate 1 being a n-type semiconductor. With the largest effective atomic number among all reported radiation-detection semiconductor materials, charge transport properties and photoconductivity were investigated under Xray excitation for 1: a large on-off ratio of 500 and considerable charge mobility lifetime product of 2.3 10 À4 cm 2 V À1 , as well as a high detection sensitivity of 23.4 mC Gy air À1 cm À2 .
We disclose the intrinsic semiconducting properties of one of the largest mixed-valent uranium clusters, [Single-crystal X-ray crystallography demonstrates that U V center is stabilized within a tetraoxo core surrounded by eight uranyl(VI) pentagonal bipyramidal centers. The oxidation states of uranium are substantiated by spectroscopic data and magnetic susceptibility measurement. Electronic spectroscopy and theory corroborate that U V species serve as electron donors and thus facilitate 1 being a n-type semiconductor. With the largest effective atomic number among all reported radiation-detection semiconductor materials, charge transport properties and photoconductivity were investigated under Xray excitation for 1: a large on-off ratio of 500 and considerable charge mobility lifetime product of 2.3 10 À4 cm 2 V À1 , as well as a high detection sensitivity of 23.4 mC Gy air À1 cm À2 .
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