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The crystal structures of (TPP) 2 [B 6 Cl 6 ](CH 3 CN) 2  and (TPP) 2 [B 6 Br 6 ](CH 3 CN) 2  were determined from single crystal X-ray diffraction analyses at 147 K. They are triclinic, space group P1̅, and contain nearly regular octahedral anions with bond lengths d(B-B) 1.716, d(B-Cl) 1.818 for [B 6 Cl 6 ] 2-  and d̅(B-B) 1.684, d̅(B-Br) 1.993 Å for [B 6 Br 6 ] 2- . Using these molecular data, normal coordinate analyses for the ten isotopomers [ 11 B n  10 B 6-n X 6 ] 2- , n = 0-6, X = Cl, Br, including the pairs of geometric isomers for n = 2, 3, 4 have been performed, based on a general valence force field. With a set of 8 force constants for Cs 2 [B 6 Br 6 ] (e.g. f d (BB) = 1.39, f d (BBr) = 3.18 mdyn/Å) and 10 for Cs 2 [B 6 Cl 16 ] (e. g. f d (BB) = 1.30, f d (BCl) = 4.01 mdyn/Å) the calculated frequencies are in good agreement with observed IR (10 K) and Raman bands (80 K) in natural abundance as well as for  11 B- and  10 B-enriched derivatives. For the series [B 6 X 6 ] 2- , X = Cl, Br, I the correlation of decreasing bond lengths d(B-B) and increasing force constants f d (BB) along with vibrational coupling between the B 6  cage and the substituent sphere is discussed.

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Kristallstrukturen von [P(C 6 H 5 ) 4 ] 2 [B 6 Cl 6 ](CH 3 CN) 2  und [P(C 6 H 5 ) 4 ] 2 [B 6 Br 6 ](CH 3 CN) 2  sowie Schwingungsspektren und Normalkoordinatenanalyse der isotopomeren closo-Hexahalogenohexaborate [ 11 B n  10 B 6-n X 6 ] 2- , Χ = Cl, Br; n = 0-6 / Crystal Structures of [P(C 6 H 5 ) 4 ] 2 [B 6 Cl 6 ](CH 3 CN) 2  and [P(C 6 H 5 ) 4 ] 2 [B 6 Br 6 ](CH 3 CN) 2 , Vibrational Spectra and Normal Coordinate Analysis of Isotopomeric closo-Hexahalogenohexaborates [ 11 B n  10 B 6-n X 6 ] 2- , X = Cl, Br; n = 0-6