Chemical composition of nanoparticles from <i>α</i>-pinene nucleation and the influence of isoprene and relative humidity at low temperature DOI Creative Commons
Lucía Caudillo, Birte Rörup, Martin Heinritzi

et al.

Atmospheric chemistry and physics, Journal Year: 2021, Volume and Issue: 21(22), P. 17099 - 17114

Published: Nov. 25, 2021

Abstract. Biogenic organic precursors play an important role in atmospheric new particle formation (NPF). One of the major precursor species is α-pinene, which upon oxidation can form a suite products covering wide range volatilities. Highly oxygenated molecules (HOMs) comprise fraction formed. While it known that HOMs contribute to secondary aerosol (SOA) formation, including NPF, they have not been well studied newly formed particles due their very low mass concentrations. Here we present gas- and particle-phase chemical composition data from experimental studies α-pinene oxidation, presence isoprene, at temperatures (−50 −30 ∘C) relative humidities (20 % 60 %) relevant upper free troposphere. The measurements took place CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber. was analyzed by thermal desorption differential mobility analyzer (TD-DMA) coupled nitrate ionization–atmospheric pressure interface–time-of-flight (CI-APi-TOF) spectrometer. CI-APi-TOF used for particle- gas-phase measurements, applying same ionization detection scheme. Our revealed C8−10 monomers C18−20 dimers as compounds (diameter up ∼ 100 nm). Particularly, system with isoprene added, C5 (C5H10O5−7) C15 (C15H24O5−10) were detected. This observation consistent previously observed such gas phase. However, although do easily nucleate, our indicate still growth tropospheric conditions. For experiments reported here, most likely enhance larger than 15 nm. Additionally, report on nucleation rates measured 1.7 nm (J1.7 nm) compared previous studies, found lower J1.7 values, higher ozone mixing ratios study.

Language: Английский

Secondary organic aerosol formed by condensing anthropogenic vapours over China’s megacities DOI
Wei Nie, Chao Yan, Dan Dan Huang

et al.

Nature Geoscience, Journal Year: 2022, Volume and Issue: 15(4), P. 255 - 261

Published: April 1, 2022

Language: Английский

Citations

154
The Synergistic Role of Sulfuric Acid, Bases, and Oxidized Organics Governing New‐Particle Formation in Beijing DOI Creative Commons
Chao Yan, Rujing Yin, Yiqun Lu

et al.

Geophysical Research Letters, Journal Year: 2021, Volume and Issue: 48(7)

Published: March 22, 2021

Abstract Intense and frequent new particle formation (NPF) events have been observed in polluted urban environments, yet the dominant mechanisms are still under debate. To understand key species governing processes of NPF we conducted comprehensive measurements downtown Beijing during January–March, 2018. We performed detailed analyses on sulfuric acid cluster composition budget, as well chemical physical properties oxidized organic molecules (OOMs). Our results demonstrate that fast clustering (H 2 SO 4 ) base triggered events, OOMs further helped grow newly formed particles toward climate‐ health‐relevant sizes. This synergistic role H , species, is likely representative environments where abundant usually co‐exist, with moderately low volatility when produced high NO x concentrations.

Language: Английский

Citations

150
Full-volatility emission framework corrects missing and underestimated secondary organic aerosol sources DOI Creative Commons
Xing Chang, Bin Zhao, Haotian Zheng

et al.

One Earth, Journal Year: 2022, Volume and Issue: 5(4), P. 403 - 412

Published: April 1, 2022

Language: Английский

Citations

120
High concentration of ultrafine particles in the Amazon free troposphere produced by organic new particle formation DOI Open Access
Bin Zhao, Manish Shrivastava, Neil M. Donahue

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2020, Volume and Issue: 117(41), P. 25344 - 25351

Published: Sept. 28, 2020

Significance The high-altitude tropics constitute one of the world’s largest aerosol reservoirs, which may significantly affect clouds, radiation, and hydrological cycle by delivering seeds on clouds form to lower altitudes maintaining stratospheric background. However, formation mechanisms these aerosols remain a scientific mystery. Through systematic experiment-based model representation organic chemistry new particle (NPF) combined with constraints from field measurements, we demonstrate that NPF driven extremely low volatility organics formed biogenic emissions plays key role in producing large number observed Amazon. This mechanism likely also prevailed during preindustrial times hence modulate anthropogenic forcing above baseline.

Language: Английский

Citations

122
Multifunctional Products of Isoprene Oxidation in Polluted Atmosphere and Their Contribution to SOA DOI Creative Commons
Zheng Xu, Wei Nie, Yuliang Liu

et al.

Geophysical Research Letters, Journal Year: 2020, Volume and Issue: 48(1)

Published: Dec. 7, 2020

Abstract Isoprene (2‐methyl‐1, 3‐butadiene) is a nonmethane volatile organic compound (VOC) with the largest global emission and high reactivity. The oxidation of isoprene crucial to atmospheric photochemistry contributes significantly formation secondary aerosol. Here, we conducted comprehensive observations in polluted megacities Nanjing Shanghai during summer 2018. We identified multiple functionalized products, which 72% 88% total mole concentration were nitrogen‐containing species dominant being C5 dihydroxyl dinitrate (C 5 H 10 N 2 O 8 ). calculated volatility using group‐contribution method estimated particle‐phase by equilibrium gas/particle partitioning. results showed that multifunctional products derived from can contribute 2.6% aerosol mass (0.28 ± 0.27 μg/m 3 ), highlighting potential importance regions.

Language: Английский

Citations

76
Atmospheric organic vapors in two European pine forests measured by a Vocus PTR-TOF: insights into monoterpene and sesquiterpene oxidation processes DOI Creative Commons
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva

et al.

Atmospheric chemistry and physics, Journal Year: 2021, Volume and Issue: 21(5), P. 4123 - 4147

Published: March 18, 2021

Abstract. Atmospheric organic vapors play essential roles in the formation of secondary aerosol. Source identification these is thus fundamental to understanding their emission sources and chemical evolution atmosphere further impact on air quality climate change. In this study, a Vocus proton-transfer-reaction time-of-flight mass spectrometer (PTR-TOF) was deployed two forested environments, Landes forest southern France boreal Finland, measure atmospheric vapors, including both volatile compounds (VOCs) oxidation products. For first time, we performed binned positive matrix factorization (binPMF) analysis complex spectra acquired with PTR-TOF identified various as well processes atmosphere. Based separate low- high-mass ranges, 15 PMF factors nine Finnish were resolved, showing high similarity between sites. Particularly, terpenes terpene reaction products separated into individual varying degrees, such lightly oxidized from monoterpene sesquiterpene oxidation, monoterpene-derived nitrates, more compounds. Factors representing monoterpenes dominated biogenic VOCs forests, lower contributions isoprene factors. products, nitrates monoterpenes/sesquiterpenes accounted for 8 %–12 % measured gas-phase forests. interpretation results relating processes, insights gained regarding reactions. example, strong relative humidity (RH) dependence found behavior High concentrations only occur at RH; yet similar not observed

Language: Английский

Citations

63
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

58
Molecular Understanding of the Enhancement in Organic Aerosol Mass at High Relative Humidity DOI Creative Commons
Mihnea Surdu, Houssni Lamkaddam, Dongyu Wang

et al.

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(6), P. 2297 - 2309

Published: Jan. 30, 2023

The mechanistic pathway by which high relative humidity (RH) affects gas–particle partitioning remains poorly understood, although many studies report increased secondary organic aerosol (SOA) yields at RH. Here, we use real-time, molecular measurements of both the gas and particle phase to provide a understanding effect RH on biogenic oxidized molecules (from α-pinene isoprene) low temperatures (243 263 K) CLOUD chamber CERN. We observe increases in SOA mass 45 85% with increasing from 10–20 60–80% 243 K, respectively, attribute it semi-volatile compounds. At measure an increase factor 2–4 concentration C10H16O2–3, while particle-phase concentrations low-volatility species, such as C10H16O6–8, remain almost constant. This results substantial shift chemical composition volatility distribution toward less oxygenated more volatile species higher (e.g., O/C ratio = 0.55 0.40, 10 80%, respectively). By modeling growth using model, accounts for kinetic limitations, can explain enhancement fraction through complementary decreased compound activity bulk-phase diffusivity. Our highlight importance water content diluting agent plasticizer growth.

Language: Английский

Citations

41
Role of sesquiterpenes in biogenic new particle formation DOI Creative Commons
Lubna Dada, Dominik Stolzenburg, Mario Simon

et al.

Science Advances, Journal Year: 2023, Volume and Issue: 9(36)

Published: Sept. 8, 2023

Biogenic vapors form new particles in the atmosphere, affecting global climate. The contributions of monoterpenes and isoprene to particle formation (NPF) have been extensively studied. However, sesquiterpenes received little attention despite a potentially important role due their high molecular weight. Via chamber experiments performed under atmospheric conditions, we report biogenic NPF resulting from oxidation pure mixtures β-caryophyllene, α-pinene, isoprene, which produces oxygenated compounds over wide range volatilities. We find that class termed ultralow-volatility organic (ULVOCs) are highly efficient nucleators quantitatively determine efficiency. When compared with mixture monoterpene alone, adding only 2% sesquiterpene increases ULVOC yield doubles rate. Thus, emissions need be included assessments aerosol concentrations pristine climates where is expected major source cloud condensation nuclei.

Language: Английский

Citations

41
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