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Polybromide monoanions of the series [NAlk4][Br9] (Alk = methyl, ethyl, propyl, butyl) have been investigated. The corresponding salts were characterized by Raman spectroscopy, single‐crystal X‐ray diffraction and state‐of‐the‐art quantum‐chemical calculations. Comparisons between their crystal structures and the gas‐phase calculations have been made whereas the latter shows regular tetrahedral arrangement...
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