From 1943 on, Booth started working on the determination of crystal structures using X-ray diffraction data.  The computations involved were extremely tedious and there was ample incentive for automating the process and he developed an analogue computer to compute the reciprocal spacings of the diffraction pattern. 
In 1947, along with his collaborator and future spouse Kathleen Britten, he spent a few months with von Neumann's team, which was the leading edge in computer research at the time.