Search for: All records

 

Abstract During near-0°C surface conditions, diverse precipitation types (p-types) are possible, including rain, drizzle, freezing rain, freezing drizzle, ice pellets, wet snow, snow, and snow pellets. Near-0°C precipitation affects wide swaths of the United States and Canada, impacting aviation, road transportation, power generation and distribution, winter recreation, ecology, and hydrology. Fundamental challenges remain in observing, diagnosing, simulating, and forecasting near-0°C p-types, particularly during transitions and within complex terrain. Motivated by these challenges, the field phase of the Winter Precipitation Type Research Multi-scale Experiment (WINTRE-MIX) was conducted from 1 February – 15 March 2022 to better understand how multiscale processes influence the variability and predictability of p-type and amount under near-0°C surface conditions. WINTRE-MIX took place near the US / Canadian border, in northern New York and southern Quebec, a region with plentiful near-0°C precipitation influenced by terrain. During WINTRE-MIX, existing advanced mesonets in New York and Quebec were complemented by deployment of: (1) surface instruments, (2) the National Research Council Convair-580 research aircraft with W- and X-band Doppler radars and in situ cloud and aerosol instrumentation, (3) two X-band dual-polarization Doppler radars and a C-band dual-polarization Doppler radar from University of Illinois, and (4) teams collecting manual hydrometeor observations and radiosonde measurements. Eleven intensive observing periods (IOPs) were coordinated. Analysis of these WINTRE-MIX IOPs is illuminating how synoptic dynamics, mesoscale dynamics, and microscale processes combine to determine p-type and its predictability under near-0°C conditions. WINTRE-MIX research will contribute to improving nowcasts and forecasts of near-0°C precipitation through evaluation and refinement of observational diagnostics and numerical forecast models. 

Abstract The interaction between nitrogen monoxide (NO) and organic peroxy radicals (RO 2 ) greatly impacts the formation of highly oxygenated organic molecules (HOM), the key precursors of secondary organic aerosols. It has been thought that HOM production can be significantly suppressed by NO even at low concentrations. Here, we perform dedicated experiments focusing on HOM formation from monoterpenes at low NO concentrations (0 – 82 pptv). We demonstrate that such low NO can enhance HOM production by modulating the RO 2 loss and favoring the formation of alkoxy radicals that can continue to autoxidize through isomerization. These insights suggest that HOM yields from typical boreal forest emissions can vary between 2.5%-6.5%, and HOM formation will not be completely inhibited even at high NO concentrations. Our findings challenge the notion that NO monotonically reduces HOM yields by extending the knowledge of RO 2 -NO interactions to the low-NO regime. This represents a major advance towards an accurate assessment of HOM budgets, especially in low-NO environments, which prevails in the pre-industrial atmosphere, pristine areas, and the upper boundary layer. 

Abstract. Highly oxygenated organic molecules (HOMs) contributesubstantially to the formation and growth of atmospheric aerosol particles,which affect air quality, human health and Earth's climate. HOMs are formedby rapid, gas-phase autoxidation of volatile organic compounds (VOCs) suchas α-pinene, the most abundant monoterpene in the atmosphere. Due totheir abundance and low volatility, HOMs can play an important role innew-particle formation (NPF) and the early growth of atmospheric aerosols,even without any further assistance of other low-volatility compounds suchas sulfuric acid. Both the autoxidation reaction forming HOMs and theirNPF rates are expected to be strongly dependent ontemperature. However, experimental data on both effects are limited.Dedicated experiments were performed at the CLOUD (Cosmics Leaving OUtdoorDroplets) chamber at CERN to address this question. In this study, we showthat a decrease in temperature (from +25 to −50 ∘C) results ina reduced HOM yield and reduced oxidation state of the products, whereas theNPF rates (J1.7 nm) increase substantially.Measurements with two different chemical ionization mass spectrometers(using nitrate and protonated water as reagent ion, respectively) providethe molecular composition of the gaseous oxidation products, and atwo-dimensional volatility basis set (2D VBS) model provides their volatilitydistribution. The HOM yield decreases with temperature from 6.2 % at 25 ∘C to 0.7 % at −50 ∘C. However, there is a strongreduction of the saturation vapor pressure of each oxidation state as thetemperature is reduced. Overall, the reduction in volatility withtemperature leads to an increase in the nucleation rates by up to 3orders of magnitude at −50 ∘C compared with 25 ∘C. Inaddition, the enhancement of the nucleation rates by ions decreases withdecreasing temperature, since the neutral molecular clusters have increasedstability against evaporation. The resulting data quantify how the interplaybetween the temperature-dependent oxidation pathways and the associatedvapor pressures affect biogenic NPF at the molecularlevel. Our measurements, therefore, improve our understanding of purebiogenic NPF for a wide range of tropospherictemperatures and precursor concentrations. 

A major fraction of atmospheric aerosol particles, which affect both air quality and climate, form from gaseous precursors in the atmosphere. Highly oxygenated organic molecules (HOMs), formed by oxidation of biogenic volatile organic compounds, are known to participate in particle formation and growth. However, it is not well understood how they interact with atmospheric pollutants, such as nitrogen oxides (NO x ) and sulfur oxides (SO x ) from fossil fuel combustion, as well as ammonia (NH 3 ) from livestock and fertilizers. Here, we show how NO x suppresses particle formation, while HOMs, sulfuric acid, and NH 3 have a synergistic enhancing effect on particle formation. We postulate a novel mechanism, involving HOMs, sulfuric acid, and ammonia, which is able to closely reproduce observations of particle formation and growth in daytime boreal forest and similar environments. The findings elucidate the complex interactions between biogenic and anthropogenic vapors in the atmospheric aerosol system.