Neutron time-of-flight diagnostics at the NIF were recently outfitted with Cherenkov detectors. A fused silica radiator delivers sub-nanosecond response time and is optically coupled to a microchannel plate photomultiplier tube with gain from ∼1 to 104. Capitalizing on fast time response and gamma-ray sensitivity, these systems can provide better than 30 ps precision for measuring first moments of neutron distributions. Generation of ab initio instrument response functions (IRFs) is critical to meet the <1% uncertainty needed. A combination of Monte Carlo modeling, benchtop characterization, and in situ comparison is employed. Close agreement is shown between the modeled IRFs and in situ measurements using the NIF's short-pulse advanced radiographic capability beams. First and second moments of neutron spectra calculated using ab initio IRFs agree well with established scintillator measurements. Next-step designs offer increased sensitivity and time-response.