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The impact of relative humidity (RH) on organic new particle formation (NPF) from ozonolysis of monoterpenes remains an area of active debate. Previous reports provide contradictory results indicating both depression and enhancement of NPF under conditions of moderate RH, while others do not indicate a potential impact. Only several reports have suggested that the effect may depend on absolute mixing ratio of the precursor volatile organic compound (VOC, ppbv). Herein we report on the impact of RH on NPF from dark ozonolysis of α- and β-pinene at mixing ratios ranging from 0.2 to 80 ppbv. We show that RH enhances NPF (by a factor of eight) at the lowest α-pinene mixing ratio, with a very strong dependence on α-pinene mixing ratio from 4 to 22 ppbv. At higher mixing ratios, the effect of RH plateaus, with resulting modest decreases in NPF. In the case of α- and β-pinene, NPF is enhanced at low mixing ratios due to a combination of chemistry, accelerated kinetics, and reduced partitioning of semi-volatile oxidation products to the particulate phase. Reduced partitioning would limit particle growth, permitting increased gas-phase concentrations of semi- and low-volatility products, which could favor NPF. 

Abstract. Secondary organic aerosol (SOA), formed through oxidation of volatile organic compounds (VOCs), displays complex viscosity and phase behaviorsinfluenced by temperature, relative humidity (RH), and chemical composition. Here, the efficacy of a multi-stage electrical low-pressure impactor(ELPI) for indirect water uptake measurements was studied for ammonium sulfate (AS) aerosol, sucrose aerosol, and α-pinene-derived SOA. Allthree aerosol systems were subjected to greater than 90 % chamber relative humidity, with subsequent analysis indicating persistence of particlebounce for sucrose aerosol of 70 nm (initial dry diameter) and α-pinene-derived SOA of number geometric mean diameters between 39 and136 nm (initial dry diameter). On the other hand, sucrose aerosol of 190 nm (initial dry diameter) and AS aerosol down to70 nm (initial dry diameter) exhibited no particle bounce at elevated RH. Partial drying of aerosol within the lower diameter ELPI impactionstages, where inherent and significant RH reductions occur, is proposed as one explanation for particle bounce persistence. 

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Absolute secondary organic aerosol (SOA) mass loading (CSOA) is a key parameter in determining partitioning of semi- and intermediate volatility compounds to the particle phase. Its impact on the phase state of SOA, however, has remained largely unexplored. In this study, systematic laboratory chamber measurements were performed to elucidate the influence of CSOA, ranging from 0.2 to 160 µg m−3, on the phase state of SOA formed by ozonolysis of various precursors, including α-pinene, limonene, cis-3-hexenyl acetate (CHA) and cis-3-hexen-1-ol (HXL). A previously established method to estimate SOA bounce factor (BF, a surrogate for particle viscosity) was utilized to infer particle viscosity as a function of CSOA. Results show that under nominally identical conditions, the maximum BF decreases by approximately 30% at higher CSOA, suggesting a more liquid phase state. With the exception of HXL-SOA (which acted as the negative control), the phase state for all studied SOA precursors varied as a function of CSOA. Furthermore, the BF was found to be the maximum when SOA particle distributions reached a geometric mean particle diameter of 50–60 nm. Experimental results indicate that CSOA is an important parameter impacting the phase state of SOA, reinforcing recent findings that extrapolation of experiments not conducted at atmospherically relevant SOA levels may not yield results that are relevant to the natural environment.