Measurements of mobility spectra of atmospheric ions with mobility between 3.37¿10-4 and 6.91¿10-8 m2/(V s), have been made at a height of 1 m above ground at different times of day at Pune (18¿ 32' N, 73¿ 51' E, 559 m above msl), India. Measurements made for a period of two days only are presented here. Observations demonstrate the presence of all three groups of ions: small, intermediate and large, each having a distinct peak in mobility at all times of day. Diurnal variations of the mobility spectrum show that ion concentrations in all the mobility ranges increase during nighttime and attain their maximum values in the early morning hours. Mobility spectra at these early morning hours suggest the possibility of the presence of ions of mobility even larger than that of 3.37¿10-4 m2/(V s). Size distribution of atmospheric aerosol particles in the radius range of 0.0023>r>0.03 μm, as computed from the mobility spectra, are bimodal in shape throughout the day on either of the two days. One peak that occurs in the nuclei mode, is always observed at 0.003 μm, while the position of the other peak which occurs in accumulation mode, changes between 0.01 and 0.03 μm, at different times of the day. The peak in accumulation mode occurs at larger radius when the peak in nuclei mode is higher. Diurnal variation of the concentration of particles (0.03>r>0.0063 μm) in accumulation mode exhibits single periodicity with a peak in the early morning and that of particles (0.002