The gas-phase molecular structure of iso-propyl(-butyl)(trichlorosilyl)phosphine has been determined using a combination of gas electron diffraction and computational methods. The structure presents a conformational challenge that required use of the SARACEN method to combine theoretical observations into the least-squares refinement process, a great advance on the techniques used to solve the structure of the parent trisilyl phosphine. Five conformers were found on the potential-energy surface for iso-propyl(-butyl)(trichlorosilyl)phosphine using the UCONGA program, and following a series of individual structure refinements a combined model with the two most abundant confirmers was evaluated. Key structural parameters () include P-Si [225.5(6) pm], Si-Cl [204.0(1) pm] and P-C [204.0(1) pm], ∠P-C-H 101.5(5)°, ∠C-C-C (iPr) 110.5(5)°, ∠C-C-C (Bu) 109.2(5)° and ∠C-P-C 105.4(5)°.
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