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The 17-electron complex (C 5 Ph 5 )Cr(CO) 3 reacts with halogens (C 6 H 5 I‚Cl 2 , Br 2 , and I 2 ) in C 6 H 6 to yield the dimeric oxidation products [(C 5 Ph 5 )Cr(µ-X)X] 2 as thermally stable solids. Reactions with other chlorinating agents similarly yield [(C 5 Ph 5 )CrCl 2 ] 2 . An X-ray crystal structure of [(C 5 Ph 5 )Cr(µ-Cl)Cl] 2 was obtained. The magnetic properties of the Cl 2 -bridged dimer have been determined and modeled using the usual isotropic Hamiltonian H ) -2JS ˆ1‚ S ˆ2, which yields J/k ) -30 K. Low-temperature (77 K) Raman spectra of solid [(C 5 Ph 5 )-CrX 2 ] 2 (X ) Cl, I) allow assignments to be made for the metal-ring and metal halogen stretching modes in the low-frequency region (<600 cm -1 ). Tetrahydrofuran (THF) cleaves these dimers to yield complexes of the form (C 5 Ph 5 )CrX 2 (THF).

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