Impacts of coagulation on the appearance time method for new particle growth rate evaluation and their corrections DOI Creative Commons
Runlong Cai, Chenxi Li, Xu‐Cheng He

et al.

Atmospheric chemistry and physics, Journal Year: 2021, Volume and Issue: 21(3), P. 2287 - 2304

Published: Feb. 16, 2021

Abstract. The growth rate of atmospheric new particles is a key parameter that determines their survival probability becoming cloud condensation nuclei and hence impact on the climate. There have been several methods to estimate particle rate. However, due coagulation measurement uncertainties, it still challenging initial particles, especially in polluted environments with high background aerosol concentrations. In this study, we explore influences appearance time method sub-3 nm particles. principle impacts retrieved are clarified via derivations. New formulae both discrete continuous spaces proposed correct for coagulation. Aerosol dynamic models used test formulae. formation urban Beijing illustrate importance considering its calculation. We show conventional needs be corrected when sink, source, non-negligible compared growth. Under simulation conditions constant concentration non-volatile vapors, agrees theoretical rates. uncorrected parameters, e.g., vapor evaporation variation concentration, may obtained method. varying average bias 1.5–3 ranges from 6 %–44 %, maximum size-dependent 150 %. During event Beijing, was accordance contributed by sulfuric acid condensation, whereas overestimated 1.5 80

Language: Английский

Frequent new particle formation over the high Arctic pack ice by enhanced iodine emissions DOI Creative Commons
Andrea Baccarini,

L. Karlsson,

Josef Dommen

et al.

Nature Communications, Journal Year: 2020, Volume and Issue: 11(1)

Published: Oct. 1, 2020

Abstract In the central Arctic Ocean formation of clouds and their properties are sensitive to availability cloud condensation nuclei (CCN). The vapors responsible for new particle (NPF), potentially leading CCN, have remained unidentified since first aerosol measurements in 1991. Here, we report that all observed NPF events from 2018 expedition driven by iodic acid with little contribution sulfuric acid. Iodic largely explains growth ultrafine particles (UFP) most events. concentration increases significantly summer towards autumn, possibly linked ocean freeze-up a seasonal rise ozone. This leads one order magnitude higher UFP autumn. Measurements residuals suggest smaller than 30 nm diameter can activate as CCN. Therefore, iodine has potential influence over Ocean.

Language: Английский

Citations

238
Role of iodine oxoacids in atmospheric aerosol nucleation DOI
Xu‐Cheng He, Yee Jun Tham, Lubna Dada

et al.

Science, Journal Year: 2021, Volume and Issue: 371(6529), P. 589 - 595

Published: Feb. 4, 2021

Faster than expected Iodine species are one of only a handful atmospheric vapors known to make new aerosol particles, which play central role in controlling the radiative forcing climate. He et al. report experimental evidence from CERN Cosmics Leaving Outdoor Droplets, or CLOUD, chamber demonstrating that iodic acid and iodous rapidly form particles can compete with sulfuric pristine regions. Science , this issue p. 589

Language: Английский

Citations

216
Contribution of Atmospheric Oxygenated Organic Compounds to Particle Growth in an Urban Environment DOI
Xiaohui Qiao, Chao Yan, Xiaoxiao Li

et al.

Environmental Science & Technology, Journal Year: 2021, Volume and Issue: 55(20), P. 13646 - 13656

Published: Sept. 29, 2021

Gas-phase oxygenated organic molecules (OOMs) can contribute substantially to the growth of newly formed particles. However, characteristics OOMs and their contributions particle rate are not well understood in urban areas, which have complex anthropogenic emissions atmospheric conditions. We performed long-term measurement gas-phase Beijing during 2018–2019 using nitrate-based chemical ionization mass spectrometry. OOM concentrations showed clear seasonal variations, with highest summer lowest winter. Correspondingly, calculated rates due condensation were summer, followed by spring, autumn, One prominent feature this environment was a high fraction (∼75%) nitrogen-containing OOMs. These contributed only 50–60% total led condensation, owing slightly higher volatility than non-nitrate By comparing observed rates, we that sulfuric acid its clusters main contributors sub-3 nm particles, significantly promoting 3–25 In wintertime Beijing, however, there missing particles above 3 nm, remain be further investigated.

Language: Английский

Citations

88
The driving factors of new particle formation and growth in the polluted boundary layer DOI Creative Commons
Mao Xiao, C. R. Hoyle, Lubna Dada

et al.

Atmospheric chemistry and physics, Journal Year: 2021, Volume and Issue: 21(18), P. 14275 - 14291

Published: Sept. 27, 2021

Abstract. New particle formation (NPF) is a significant source of atmospheric particles, affecting climate and air quality. Understanding the mechanisms involved in urban aerosols important to develop effective mitigation strategies. However, NPF rates reported polluted boundary layer span more than 4 orders magnitude, reasons behind this variability are subject intense scientific debate. Multiple vapours have been postulated participate NPF, including sulfuric acid, ammonia, amines organics, but their relative roles remain unclear. We investigated CLOUD chamber using mixtures anthropogenic that simulate conditions. demonstrate environments largely driven by acid–base clusters, stabilized presence amines, high ammonia concentrations lower temperatures. Aromatic oxidation products, despite extremely low volatility, play minor role chosen environment can be for growth hence survival newly formed particles. Our measurements quantitatively account highly diverse explain its large observed variability. Such quantitative information obtained under controlled laboratory conditions will help interpretation future ambient observations atmospheres.

Language: Английский

Citations

78
Synergistic HNO3–H2SO4–NH3 upper tropospheric particle formation DOI Creative Commons
Mingyi Wang, Mao Xiao, Barbara Bertozzi

et al.

Nature, Journal Year: 2022, Volume and Issue: 605(7910), P. 483 - 489

Published: May 18, 2022

Abstract New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN) 1–4 . However, precursor vapours that drive process are not well understood. With experiments performed under tropospheric conditions CERN CLOUD chamber, we show nitric acid, sulfuric acid and ammonia form particles synergistically, at rates orders magnitude faster than those from any two three components. The importance this mechanism depends on availability ammonia, which was previously thought to be efficiently scavenged by droplets during convection. surprisingly high concentrations ammonium nitrate have recently been observed over Asian monsoon region 5,6 Once formed, co-condensation abundant alone sufficient rapid growth CCN sizes with only trace sulfate. Moreover, our measurements these also highly efficient ice nucleating particles—comparable desert dust. Our model simulations confirm convected aloft monsoon, driving rapid, multi-acid HNO 3 –H 2 SO 4 –NH nucleation producing spread across mid-latitude Northern Hemisphere.

Language: Английский

Citations

59
The missing base molecules in atmospheric acid–base nucleation DOI Creative Commons
Runlong Cai, Rujing Yin, Chao Yan

et al.

National Science Review, Journal Year: 2022, Volume and Issue: 9(10)

Published: July 25, 2022

Transformation of low-volatility gaseous precursors to new particles affects aerosol number concentration, cloud formation and hence the climate. The clustering acid base molecules is a major mechanism driving fast nucleation initial growth in atmosphere. However, acid-base cluster composition, measured using state-of-the-art mass spectrometers, cannot explain high rate particles. Here we present strong evidence for existence such as amines smallest atmospheric sulfuric clusters prior their detection by spectrometers. We demonstrate that forming (H2SO4)1(amine)1 rate-limiting step H2SO4-amine uptake pathway H2SO4 clusters. proposed very consistent with particle urban Beijing, which dimethylamine key while other bases ammonia may contribute larger Our findings further underline fact amines, even at low concentrations when undetected clusters, can be crucial planetary boundary layer.

Language: Английский

Citations

48
Iodine oxoacids enhance nucleation of sulfuric acid particles in the atmosphere DOI Open Access
Xu‐Cheng He, Mario Simon, Siddharth Iyer

et al.

Science, Journal Year: 2023, Volume and Issue: 382(6676), P. 1308 - 1314

Published: Dec. 14, 2023

The main nucleating vapor in the atmosphere is thought to be sulfuric acid (H2SO4), stabilized by ammonia (NH3). However, marine and polar regions, NH3 generally low, H2SO4 frequently found together with iodine oxoacids [HIOx, i.e., iodic (HIO3) iodous (HIO2)]. In experiments performed CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we investigated interplay of HIOx during atmospheric particle nucleation. We that greatly enhances H2SO4(-NH3) nucleation through two different interactions. First, HIO3 strongly binds charged clusters so they drive synergistically. Second, HIO2 substitutes for NH3, forming bound H2SO4-HIO2 acid-base pairs molecular clusters. Global observations imply enhancing rates 10- 10,000-fold regions.

Language: Английский

Citations

40
Significant contributions of trimethylamine to sulfuric acid nucleation in polluted environments DOI Creative Commons
Runlong Cai, Rujing Yin, Xue Li

et al.

npj Climate and Atmospheric Science, Journal Year: 2023, Volume and Issue: 6(1)

Published: June 27, 2023

Abstract As one of the least understood aerosol processes, nucleation can be a dominant source atmospheric aerosols. Sulfuric acid (SA)-amine binary with dimethylamine (DMA) has been recognized as governing mechanism in polluted continental boundary layer. Here we demonstrate importance trimethylamine (TMA) for complex atmosphere and propose molecular-level SA-DMA-TMA ternary an improvement upon conventional mechanism. Using proposed mechanism, could connect gaseous amines to SA-amine cluster signals measured urban Beijing. Results show that TMA accelerate SA-DMA-based new particle formation Beijing by 50–100%. Considering global abundance DMA, our findings imply comparable DMA layer, probably higher contributions from rural environments future controlled emissions.

Language: Английский

Citations

31
Atmospheric new particle formation from the CERN CLOUD experiment DOI
J. Kirkby, A. Amorim, Urs Baltensperger

et al.

Nature Geoscience, Journal Year: 2023, Volume and Issue: 16(11), P. 948 - 957

Published: Nov. 1, 2023

Language: Английский

Citations

29
Quantum chemical modeling of organic enhanced atmospheric nucleation: A critical review DOI Creative Commons
Jonas Elm, Daniel Ayoubi, Morten Engsvang

et al.

Wiley Interdisciplinary Reviews Computational Molecular Science, Journal Year: 2023, Volume and Issue: 13(5)

Published: May 9, 2023

Abstract Aerosol particles are important for our global climate, but the mechanisms and especially relative importance of various vapors new formation (NPF) remain uncertain. Quantum chemical (QC) studies on organic enhanced nucleation has past couple decades attracted immense attention, very little remains known about exact compounds that potentially NPF. Here we comprehensively review QC literature atmospheric cluster involving compounds. We outline potential systems should be further investigated. Cluster complex multi‐functional accretion products warrant investigations, such out reach with currently applied methodologies. suggest a “cluster functional groups” approach to address this issue, which will allow identification structure involved in This article is categorized under: Theoretical Physical Chemistry > Reaction Dynamics Kinetics Software Thermochemistry Molecular Statistical Mechanics Interactions

Language: Английский

Citations

26