An official website of the United States government
Abstract. New particle formation (NPF) consists of two steps: nucleation andsubsequent growth. At present, chemical and physical mechanisms that governthese two processes are not well understood. Here, we report initial resultsobtained from the TANGENT (Tandem Aerosol Nucleation and Growth EnvironmentTube) experiments. The TANGENT apparatus enables us to study these twoprocesses independently. The present study focuses on the effects oftemperature on sulfuric acid nucleation and further growth. Our results showthat lower temperatures enhance both the nucleation and growth rate.However, under temperatures below 268 K the effects of temperature on thenucleation rate become less significant and the nucleation rate becomes lessdependent on relative humidity, indicating that particle formation in the conditions of ourflow tube takes place via barrierless nucleation at lower temperatures. Wealso examined the growth of newly formed particles under differingtemperature conditions for nucleation and further growth. Our results showthat newly nucleated clusters formed at low temperatures can indeed surviveevaporation and grow in a warmer environment in the presence of SO2 andozone and potentially other contaminant vapors. These results implythat some heterogeneous reactions involving nanoparticles affect nucleationand growth of newly formed particles.
more »
« less
New Particle Formation in the Atmosphere: From Molecular Clusters to Global Climate
Abstract New particle formation (NPF) represents the first step in the complex processes leading to formation of cloud condensation nuclei. Newly formed nanoparticles affect human health, air quality, weather, and climate. This review provides a brief history, synthesizes recent significant progresses, and outlines the challenges and future directions for research relevant to NPF. New developments include the emergence of state‐of‐the‐art instruments that measure prenucleation clusters and newly nucleated nanoparticles down to about 1 nm; systematic laboratory studies of multicomponent nucleation systems, including collaborative experiments conducted in the Cosmics Leaving Outdoor Droplets chamber at CERN; observations of NPF in different types of forests, extremely polluted urban locations, coastal sites, polar regions, and high‐elevation sites; and improved nucleation theories and parameterizations to account for NPF in atmospheric models. The challenges include the lack of understanding of the fundamental chemical mechanisms responsible for aerosol nucleation and growth under diverse environments, the effects of SO2and NOxon NPF, and the contribution of anthropogenic organic compounds to NPF. It is also critical to develop instruments that can detect chemical composition of particles from 3 to 20 nm and improve parameterizations to represent NPF over a wide range of atmospheric conditions of chemical precursor, temperature, and humidity.
more »
« less
- Award ID(s):
- 1649694
- PAR ID:
- 10460162
- Publisher / Repository:
- DOI PREFIX: 10.1029
- Date Published:
- Journal Name:
- Journal of Geophysical Research: Atmospheres
- Volume:
- 124
- Issue:
- 13
- ISSN:
- 2169-897X
- Page Range / eLocation ID:
- p. 7098-7146
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract A key challenge in aerosol pollution studies and climate change assessment is to understand how atmospheric aerosol particles are initially formed1,2. Although new particle formation (NPF) mechanisms have been described at specific sites3–6, in most regions, such mechanisms remain uncertain to a large extent because of the limited ability of atmospheric models to simulate critical NPF processes1,7. Here we synthesize molecular-level experiments to develop comprehensive representations of 11 NPF mechanisms and the complex chemical transformation of precursor gases in a fully coupled global climate model. Combined simulations and observations show that the dominant NPF mechanisms are distinct worldwide and vary with region and altitude. Previously neglected or underrepresented mechanisms involving organics, amines, iodine oxoacids and HNO3probably dominate NPF in most regions with high concentrations of aerosols or large aerosol radiative forcing; such regions include oceanic and human-polluted continental boundary layers, as well as the upper troposphere over rainforests and Asian monsoon regions. These underrepresented mechanisms also play notable roles in other areas, such as the upper troposphere of the Pacific and Atlantic oceans. Accordingly, NPF accounts for different fractions (10–80%) of the nuclei on which cloud forms at 0.5% supersaturation over various regions in the lower troposphere. The comprehensive simulation of global NPF mechanisms can help improve estimation and source attribution of the climate effects of aerosols.more » « less
-
Abstract New particle formation (NPF) is a complex atmospheric phenomenon defined by the gas‐to‐particle conversion that leads to the sudden burst and growth in aerosol particles. Although chemical mechanisms for aerosol nucleation and growth are well established, the role of physical processes, such as turbulent mixing, within the atmospheric boundary layer (ABL) is beginning to emerge with recent studies. This study, based on the observations from the 2022 CFACT (Cold Fog Amongst Complex Terrain) field study in the Heber Valley of northern Utah, demonstrates an interconnection between turbulence and the occurrence of NPF. Using a spatially distributed boundary layer instrumentation, a novel feature of CFACT, three case studies depict unique boundary layer conditions that modulate the development of NPF characterized by sustained turbulence and weak intermittent turbulence. Quantitative analysis using in situ measurements and derived variables demonstrate that periods of weak intermittent turbulence hinder particle growth, whereas sustained turbulence helps modulate NPF. These findings provide new insights into the physical drivers of NPF, underscoring the role of turbulence in impacting particle formation with the ABL.more » « less
-
Reduced-nitrogen compounds (RNC), such as ammonia and amines, play important roles in atmospheric aerosol nucleation, secondary organic aerosol (SOA), and cloud formation processes. Fast measurements of ammonia and amines are made with a chemical ionization mass spectrometer (CIMS). Clusters containing RNC are measured with an atmospheric pressure interface time of flight mass spectrometer (APi-TOF) or chemical ionization APi-TOF (CI-APi-TOF). Aerosol-phase amines can be detected with a single particle mass spectrometer at real-time, or with offline chemical analytical methods using filter samples. However, the application of these instruments in real atmospheric measurements is still very limited. This perspective article highlights recent measurements of RNC in the atmosphere and discusses their implications in new particle formation (NPF).more » « less
-
The energy landscape is changing worldwide, with a drastic reduction in sulfur dioxide (precursor to sulfuric acid, H2SO4) emitted from fossil fuel combustion. As a result, acid-base chemistry leading to new particle formation (NPF) from sulfuric acid is decreasing. At the same time, photooxidation of biogenic organosulfur compounds leading to the formation of H2SO4 and methanesulfonic acid (MSA) is expected to become more important. Aqueous solutions of alkanolamines have been proposed as carbon capture technology media to store carbon dioxide from stack plumes before release into the atmosphere. It is therefore expected that some of the alkanolamines will be released, making it critical to understand their atmospheric fates including their role in new particle formation and growth. We expanded our experimental studies of nucleation from the reaction of MSA with simple amines to the multifunctional alkanolamines, including mononethanolamine (HO(CH2)2NH2; MEA) and 4-aminobutanol (HO(CH2)4NH2; 4AB). Experiments were performed in a 1-m borosilicate flow reactor under dry conditions as well as in presence of water. These two systems were shown to produce sub-10 nm particles with MSA extremely efficiently. Surprisingly, the presence of water did not enhance NPF, in contrast to the drastic effect water had on small alkylamine reactions with MSA. This is likely due to the fact that MEA and 4AB have an -OH group that provides additional H-bond interactions within the cluster. Sampling of the chemical composition of these small nanoparticles with high resolution and high transmission was possible down to 3-4 nm using a novel high-flow differential mobility analyzer (half-mini DMA) interfaced to a thermal chemical ionization mass spectrometer (TDCIMS). There was no size dependence for the acid-to-base molar ratio (1:1) for either amine. Integration of these data with preliminary results obtained for a simple C4 alkylamine (butylamine) and a C4 diamine (putrescine) will be discussed in the context of developing a molecular structure-reactivity scheme for new particle formation from MSA and amines of varying structures.more » « less
