The reaction of [(c-C6H11)7Si7O9(OSiMe3)(OTl)2] with [Mo(CHCMe2Ph)(NAr)(OSO2CF3)2(dme)] (Ar=2,6-diisopropylphenyl) affords 4a as the predominant (>99%) molybdenum-containing product. Assignment of 4a as the syn-isomer with juxtaposed arylimido and Me3Si groups was made on the basis of double pulsed field gradient spin echo (DPFGSE) NOE experiments and confirmed by a single-crystal x-ray diffraction study.