The positive ion mass spectrometer on the Geoprobe (NASA 8.25) rocket measured the concentrations of O+, N+, H+, He+, NO+, O2+ and N2+ between 200 km and peak altitude, 630 km, at 1300 EST on March 2, 1966, above Wallops Island, Virginia. The dominant ion throughout the altitude range was O+, with a maximum concentration of 5 × 105 ions/cm³ at 260 km. The first detection of H+ occurred at 230 km, its concentration increasing to 7 × 10³ ions/cm³ at peak altitude. The H+/He+ ratio was never lower than 6.0, the value at 420 km. The molecular ions NO+ and O2+ were important constituents at 200 km, the concentration of each being 5 × 104 ions/cm³; they fell off rapidly above this altitude. Photochemical equilibrium held for He+ up to 400 km with a rate coefficient of about 0.5 × 10−9 cm³ sec−1 for charge transfer with N2, in agreement with laboratory measurement. Charge exchange equilibrium of H+ with O+, O, and H held up to 350 km; the temperature derived for the neutrals below 350 km, where it is believed that Tg = Ti, was 850°K, which agrees with Tg measured by companion neutral particle sensors. From the variation of [H+]/[O+] and an [O] distribution based on a simultaneous EUV measurement, a profile of [H] in the chemical equilibrium region was calculated. The derived H concentrations are higher than the Jacchia 1964 Model predictions, but agree with Explorer 32 spectrometer results. Analysis indicates that N+ was not in diffusive equilibrium at 300 km, and that a neutral wind having a field-aligned downward component of 25 m/sec is required to produce the observed N+ scale height at this altitude. Distributions of O+ and H+ above 300 km were derived by solving the continuity equations along field lines; an upward H+ flux of 1.5 × 108/cm² sec was required to reproduce the observed profiles, indicating that the critical flux is at least an order of magnitude higher than previously believed.