Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures DOI Creative Commons
Andreas Kürten, Federico Bianchi, J. Almeida

et al.

Journal of Geophysical Research Atmospheres, Journal Year: 2016, Volume and Issue: 121(20)

Published: Oct. 27, 2016

Abstract Binary nucleation of sulfuric acid and water as well ternary involving ammonia are thought to be the dominant processes responsible for new particle formation (NPF) in cold temperatures middle upper troposphere. Ions also important these regions. However, global models presently lack experimentally measured NPF rates under controlled laboratory conditions so at present must rely on theoretical or empirical parameterizations. Here with data obtained European Organization Nuclear Research CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we first experimental survey spanning free tropospheric conditions. The during cover a temperature range from 208 298 K, concentrations between 5 × 10 1 9 cm −3 , mixing ratios zero added ammonia, i.e., nominally pure binary, maximum ~1400 parts per trillion by volume (pptv). We performed studies neutral ions being chamber ionization up 75 ion pairs s −1 study ion‐induced nucleation. found that contribution is small 248 K when several pptv higher. presence charges significantly enhances rates, especially higher independent NH 3 levels. compare calculated cluster Atmospheric Cluster Dynamics Code evaporation quantum chemistry.

Language: Английский

Atmospheric new particle formation from sulfuric acid and amines in a Chinese megacity DOI Open Access
Lei Yao, Olga Garmаsh, Federico Bianchi

et al.

Science, Journal Year: 2018, Volume and Issue: 361(6399), P. 278 - 281

Published: July 19, 2018

Atmospheric new particle formation (NPF) is an important global phenomenon that nevertheless sensitive to ambient conditions. According both observation and theoretical arguments, NPF usually requires a relatively high sulfuric acid (H2SO4) concentration promote the of particles low preexisting aerosol loading minimize sink particles. We investigated in Shanghai were able observe precursor vapors initial clusters at molecular level megacity. High rates observed coincide with several familiar markers suggestive H2SO4-dimethylamine (DMA)-water (H2O) nucleation, including dimers H2SO4-DMA clusters. In cluster kinetics simulation, was enough explain growth ~3 nanometers under very condensation sink, whereas subsequent higher rate beyond this size believed result from added contribution condensing organic species. These findings will help understanding urban its air quality climate effects, as well formulating policies mitigate secondary China.

Language: Английский

Citations

660
Aerosol Health Effects from Molecular to Global Scales DOI
Manabu Shiraiwa, Kayo Ueda, Andrea Pozzer

et al.

Environmental Science & Technology, Journal Year: 2017, Volume and Issue: 51(23), P. 13545 - 13567

Published: Nov. 7, 2017

Poor air quality is globally the largest environmental health risk. Epidemiological studies have uncovered clear relationships of gaseous pollutants and particulate matter (PM) with adverse outcomes, including mortality by cardiovascular respiratory diseases. Studies impacts aerosols are highly multidisciplinary a broad range scales in space time. We assess recent advances future challenges regarding aerosol effects on from molecular to global through epidemiological studies, field measurements, health-related properties PM, multiphase interactions oxidants PM upon deposition. Global modeling combined exposure-response functions indicates that ambient pollution causes more than four million premature deaths per year. usually refer mass concentrations, but some may relate specific constituents such as bioaerosols, polycyclic aromatic compounds, transition metals. Various analytical techniques cellular assays applied redox activity formation reactive oxygen species. Multiphase chemical lung antioxidants atmospheric crucial mechanistic understanding oxidative stress The role distinct components needs be clarified integrated research various spatiotemporal for better evaluation mitigation public Anthropocene.

Language: Английский

Citations

611
Atmospheric new particle formation and growth: review of field observations DOI Creative Commons
Veli‐Matti Kerminen, Xuemeng Chen,

Ville Vakkari

et al.

Environmental Research Letters, Journal Year: 2018, Volume and Issue: 13(10), P. 103003 - 103003

Published: Sept. 6, 2018

This review focuses on the observed characteristics of atmospheric new particle formation (NPF) in different environments global troposphere. After a short introduction, we will present theoretical background that discusses methods used to analyze measurement data NPF and associated terminology. We update our current understanding regional NPF, i.e. taking simultaneously place over large spatial scales, complement with full reported growth rates during events. shortly at sub-regional scales. Since newly-formed particles into larger sizes is great interest, briefly discuss observation-based which gaseous compounds contribute particles, what implications this have cloud condensation nuclei formation. finish summary main findings future outlook outlines remaining research questions needs for additional measurements.

Language: Английский

Citations

610
Solar forcing for CMIP6 (v3.2) DOI Creative Commons
Katja Matthes, B. Funke,

M. E. Andersson

et al.

Geoscientific model development, Journal Year: 2017, Volume and Issue: 10(6), P. 2247 - 2302

Published: June 22, 2017

Abstract. This paper describes the recommended solar forcing dataset for CMIP6 and highlights changes with respect to CMIP5. The is provided radiative properties, namely total irradiance (TSI), spectral (SSI), F10.7 index as well particle forcing, including geomagnetic indices Ap Kp, ionization rates account effects of protons, electrons, galactic cosmic rays. first time that a recommendation solar-driven has been CMIP exercise. datasets are at daily monthly resolution separately preindustrial control, historical (1850–2014), future (2015–2300) simulations. For control simulation, both constant time-varying components provided, latter variability on 11-year shorter timescales but no long-term changes. future, we provide realistic scenario what behavior could be, an additional extreme Maunder-minimum-like sensitivity scenario. also provides detailed recommendations their implementation in current climate models.For simulations, TSI SSI series defined average two models adapted needs: empirical one (NRLTSI2–NRLSSI2) semi-empirical (SATIRE). A new lower value recommended: contemporary solar-cycle now 1361.0 W m−2. slight negative trend over three most recent cycles leads only small global −0.04 In 200–400 nm wavelength range, which important ozone photochemistry, shows larger contribution than CMIP5 (50 % compared 35 %).We compare climatic its predecessor by using time-slice experiments chemistry–climate reference transfer model. differences mean dataset, CMIP5, impact climatological stratospheric conditions (lower shortwave heating −0.35 K day−1 stratopause), cooler temperatures (−1.5 upper stratosphere), abundances stratosphere (−3 %), higher (+1.5 mesosphere). Between maximum minimum phases cycle, there increase (+0.2 ( ∼ 1 (+2.5 stratosphere) tropical dataset. response slightly larger, not statistically significantly different from dataset.CMIP6 well-resolved radiation scheme encouraged prescribe include solar-induced variations, order better represent and/or exclude solar-ozone response. We show monthly-mean variations implicitly included SPARC/CCMI Ozone Database derived transient model simulations developed do calculate interactively. without chemistry perform simulation will need use modified version includes variability. interactive datasets, allow potential particles be addressed time. consideration shown improve representation reactive nitrogen polar middle atmosphere, eventually resulting further improvements models.

Language: Английский

Citations

455
Causes and importance of new particle formation in the present‐day and preindustrial atmospheres DOI Creative Commons
Hamish Gordon, J. Kirkby, Urs Baltensperger

et al.

Journal of Geophysical Research Atmospheres, Journal Year: 2017, Volume and Issue: 122(16), P. 8739 - 8760

Published: July 10, 2017

Abstract New particle formation has been estimated to produce around half of cloud‐forming particles in the present‐day atmosphere, via gas‐to‐particle conversion. Here we assess importance new (NPF) for both and preindustrial atmospheres. We use a global aerosol model with parametrizations NPF from previously published CLOUD chamber experiments involving sulfuric acid, ammonia, organic molecules, ions. find that produces 67% cloud condensation nuclei at 0.2% supersaturation (CCN0.2%) level low clouds atmosphere (estimated uncertainty range 45–84%) 54% present day 38–66%). Concerning causes, biogenic volatile compounds (BVOCs) CCN is greater than thought. Removing BVOCs hence all secondary our reduces low‐cloud‐level concentrations by 26% 41% preindustrial. Around three quarters this reduction due tiny fraction oxidation products have sufficiently volatility be involved early growth. Furthermore, estimate 40% CCN0.2% are formed ion‐induced NPF, compared 27% day, although caution poorly measured present. Our suggests effect changes cosmic ray intensity on small unlikely comparable large variations natural primary emissions.

Language: Английский

Citations

443
New Particle Formation in the Atmosphere: From Molecular Clusters to Global Climate DOI Creative Commons
Shan‐Hu Lee, Hamish Gordon, Huan Yu

et al.

Journal of Geophysical Research Atmospheres, Journal Year: 2019, Volume and Issue: 124(13), P. 7098 - 7146

Published: June 25, 2019

Abstract New particle formation (NPF) represents the first step in complex processes leading to 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, outlines challenges future directions for research relevant NPF. developments include emergence state‐of‐the‐art instruments that measure prenucleation clusters newly nucleated down about 1 nm; systematic laboratory studies multicomponent nucleation systems, including collaborative experiments conducted Cosmics Leaving Outdoor Droplets chamber at CERN; observations NPF different types forests, extremely polluted urban locations, coastal sites, polar regions, high‐elevation sites; improved theories parameterizations account atmospheric models. The lack understanding fundamental chemical mechanisms responsible aerosol growth under diverse environments, effects SO 2 NO x on NPF, contribution anthropogenic organic compounds It is also critical develop can detect composition particles from 3 20 nm improve represent over wide range conditions precursor, temperature, humidity.

Language: Английский

Citations

366
Multicomponent new particle formation from sulfuric acid, ammonia, and biogenic vapors DOI Creative Commons
Katrianne Lehtipalo, Chao Yan, Lubna Dada

et al.

Science Advances, Journal Year: 2018, Volume and Issue: 4(12)

Published: Dec. 7, 2018

Atmospheric aerosol formation from biogenic vapors is strongly affected by air pollutants, like NO x , SO 2 and NH 3 .

Language: Английский

Citations

315
A large source of cloud condensation nuclei from new particle formation in the tropics DOI
Christina Williamson,

Agnieszka Kupc,

Duncan Axisa

et al.

Nature, Journal Year: 2019, Volume and Issue: 574(7778), P. 399 - 403

Published: Oct. 16, 2019

Language: Английский

Citations

242
Differing Mechanisms of New Particle Formation at Two Arctic Sites DOI Creative Commons
Lisa Beck, Nina Sarnela, Heikki Junninen

et al.

Geophysical Research Letters, Journal Year: 2020, Volume and Issue: 48(4)

Published: Dec. 29, 2020

Abstract New particle formation in the Arctic atmosphere is an important source of aerosol particles. Understanding processes secondary crucial due to their significant impact on cloud properties and therefore amplification. We observed molecular new particles from low‐volatility vapors at two sites with differing surroundings. In Svalbard, sulfuric acid (SA) methane sulfonic (MSA) contribute some extent condensation nuclei (CCN). This occurs via ion‐induced nucleation SA NH 3 subsequent growth by mainly MSA during springtime highly oxygenated organic molecules summertime. By contrast, ice‐covered region around Villum, we driven iodic but its concentration was insufficient grow nucleated CCN sizes. Our results provide insight about sources precursors

Language: Английский

Citations

241
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