Tethered balloon system and High-Resolution Mass Spectrometry Reveal Increased Organonitrates Aloft Compared to the Ground Level.

Atmospheric particles play critical roles in climate. However, significant knowledge gaps remain regarding the vertically resolved organic molecular-level composition of atmospheric particles due to aloft sampling challenges. To address this, we use a tethered balloon system at the Southern Great Plains Observatory and high-resolution mass spectrometry to, respectively, collect and characterize organic molecular formulas (MF) in the ground level and aloft (up to 750 m) samples. We show that organic MF uniquely detected aloft were dominated by organonitrates (139 MF; 54% of all uniquely detected aloft MF). Organonitrates that were uniquely detected aloft featured elevated O/C ratios (0.73 ± 0.23) compared to aloft organonitrates that were commonly observed at the ground level (0.63 ± 0.22). Unique aloft organic molecular composition was positively associated with increased cloud coverage, increased aloft relative humidity (∼40% increase compared to ground level), and decreased vertical wind variance. Furthermore, 29% of extremely low volatility organic compounds in the aloft sample were truly unique to the aloft sample compared to the ground level, emphasizing potential oligomer formation at higher altitudes. Overall, this study highlights the importance of considering vertically resolved organic molecular composition (particularly for organonitrates) and hypothesizes that aqueous phase transformations and vertical wind variance may be key variables affecting the molecular composition of aloft organic aerosol.

Vertical Gradient of Size-Resolved Aerosol Compositions over the Arctic Reveals Cloud Processed Aerosol in-Cloud and above Cloud.

Arctic aerosols play a significant role in aerosol-radiation and aerosol-cloud interactions, but ground-based measurements are insufficient to explain the interaction of aerosols and clouds in a vertically stratified Arctic atmosphere. This study shows the vertical variability of a size resolved aerosol composition via a tethered balloon system at Oliktok Point, Alaska, at different cloud layers for two representative case studies (background aerosol and polluted conditions). Multimodal microspectroscopy analysis during the background case reveals a broadening of chemically specific size distribution above the cloud top with a high abundance of sulfate particles and core-shell morphology, suggesting possible cloud processing of aerosols. The polluted case also indicates broadening of aerosol size distribution at the upper layer within the clouds with the dominance of carbonaceous particles, which suggests that the carbonaceous particles play a potential role in modulating Arctic cloud properties.

Performance Assessment of Portable Optical Particle Spectrometer (POPS).

Accurate representation of atmospheric aerosol properties is a long-standing problem in atmospheric research. Modern pilotless aerial systems provide a new platform for atmospheric in situ measurement. However, small airborne platforms require miniaturized instrumentation due to apparent size, power, and weight limitations. A Portable Optical Particle Spectrometer (POPS) is an emerged instrument to measure ambient aerosol size distribution with high time and size resolution, designed for deployment on a small unmanned aerial system (UAS) or tethered balloon system (TBS) platforms. This study evaluates the performance of a POPS with an upgraded laser heater and additional temperature sensors in the aerosol pathway. POPS maintains its performance under different environmental conditions as long as the laser temperature remains above 25 °C and the aerosol flow temperature inside the optical chamber is 15 °C higher than the ambient temperature. The comparison between POPS and an Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) suggests that the coincidence error is less than 25% when the number concentration is less than 4000 cm-3. The size distributions measured by both of them remained unaffected up to 15,000 cm-3. While both instruments' sizing accuracy is affected by the aerosol chemical composition and morphology, the influence is more profound on the POPS.