Atmospheric acidity as HNO,(g), SO,(g), and aerosol H + was measured on Allegheny Mountain and Laurel Hill in southwest Pennsylvania in August 1983. The aerosol H+ appeared to represent the net after H,SO, reaction with NH,(g). The resulting H+/SO:-ratio depended on SOi-concentration, approaching that of H,SO, at the highest SOi-concentrations. The atmosphere was acidic; the average concentrations of HNO, (78 nmolem-3) and aerosol H+ (205 nmolem-3), NH: (172 nmolem-") and SOi-(201 nmolem-s), and the dearth of NH,(< 15 nmoleme3), show that the proton acidity (HNO,, H2S04) of the air exceeded the acid-neutralizing capacity of the air by a factor of >2, with one l&h period averaging 263 and 844 nmoleme3 for HNO, and aerosol H+, respectively. SO, added another 900 nmole mm3 (average) of potential H+ acidity. HNO, and aerosol Hf episodes were concurrent, on 7-8 day cycles, unrelated to SOi which existed m&e in short-lived bursts of apparently more local origin. NOi was sporadic like SO,. Laurel and Allegheny, separated by 35.5 km, were essentially identical in aerosol SO:-, and in aerosol H+, less so in HNO, and especially less so in SO,; apparently, chemistry involving HNO, and aerosol H+ or SOi-was slow compared to inter-site transport times (l-2 h). From growth of b,,,, and decline of SO2 during one instance of inter-site transport, daytime rate coefficients for SO, oxidation and SO, dry deposition were inferred to have been, respectively, _ 0.05 and < 0.1 h-'. HNO, declined at night. Aerosol H+ and SOi-showed no significant diurnal variation, and 0, showed very little; these observations, together with high PAN/NO, ratios, indicate that regional transport rather than local chemistry is governing. The 0, concentration (average 56 ppb or 2178 nmole m-") connotes an oxidizing atmosphere conducive to acid formation. Highest atmospheric acidity was associated with (1) slow westerly winds traversing westward SO, source areas, (2) local stagnation, or (3) regional transport around to the back side of a high pressure system. Low acidity was associated with fast-moving air masses and with winds from the northerly directions; upwind precipitation also played a moderating role in air parcel acidity. Much of the SO, and NO,, and ultimately of the HNO, and aerosol H+, appeared to originate from coal-fired power plants. An automotive contribution to the NO, and HNO, could not be discerned. Size distributions of aerosol H+ and SO:-were alike, with MMED * 0.7 pm, in the optimum range for efficient light scattering and inefficient wet/dry removal. Thus, light scattering and visual range degradation were attributable to the acidic SOi-aerosol, linking the issues of acid deposition and visual air quality in the Northeast. With inefficient removal of aerosol H+, and inefficient night-time removal of HNO,, strong acids may be capable of long-distance transport in the lower troposphere. We obtained an accounting of aerosol mass in terms of composition, including aerosol H,O which was shown to account for much of the light scattering.