The first global atmospheric model (WACCM-Al) of meteor-ablated aluminum was constructed from three components: the Whole Atmospheric Community Climate Model (WACCM6); a meteoric input function for Al derived by coupling an astronomical model of dust sources in the solar system with a chemical meteoric ablation model; and a comprehensive set of neutral, ion-molecule and photochemical reactions relevant to the chemistry of Al in the upper atmosphere. The reaction kinetics of two important reactions that control the rate at which Al⁺ ions are neutralized were first studied using a fast flow tube with pulsed laser ablation of an Al target, yielding k(AlO⁺ + CO) = (3.7 ± 1.1) × 10^-10 and k(AlO⁺ + O) = (1.7 ± 0.7) × 10^-10 cm³ molecule^-1 s^-1 at 294 K. The first attempt to observe AlO by lidar was made by probing the bandhead of the B²Σ⁺(v’ = 0) ← X²Σ⁺(v” = 0) transition at λ_air = 484.23 nm. An upper limit for AlO of 57 cm^-3 was determined, which is consistent with a night-time concentration of ~5 cm^-3 estimated from the decay of AlO following rocket-borne grenade releases. WACCM-Al predicts the following: AlO, AlOH and Al⁺ are the three major species above 80 km; the AlO layer at mid-latitudes peaks at 89 km with a half-width of ~5 km, and a peak density which increases from a night-time minimum of ~10 cm^-3 to a daytime maximum of ~60 cm^‑3; and that the best opportunity for observing AlO is at high latitudes during equinoctial twilight.