Reply on RC2 DOI Creative Commons
Giancarlo Ciarelli

Published: Sept. 12, 2023

Abstract. We present an evaluation of the regional chemical transport model (CTM) WRF-CHIMERE (v2020r2) for formation biogenic secondary organic aerosol (BSOA) with a focus over Finnish boreal forest. Formation processes aerosols are still affected by different sources uncertainties, and model’s predictions largely varies depending on levels details adopted emissions schemes. In this study, air quality simulations were conducted astronomical summer year 2019 using (OA) schemes (as currently available in literature) to treat BSOA. First, we performed set framework volatility basis (VBS) scheme carrying assumptions treatment aging The results compared against high-resolution (i.e., 1-hour) mass size distribution measurements at Station Measuring Ecosystem–Atmosphere Relations (SMEAR-II) site located Hyytiälä, addition other gas-phases species such as ozone (O3), nitrogen oxides (NOx) BVOCs isoprene (C5H10) monoterpenes. show that could well reproduce diurnal variation measured OA concentrations all investigated scenarios (along standard meteorological parameters) increase during specific heat waves episodes. However, modeled varied between use describe Additionally, comparisons monoterpenes revealed captured observed concentrations, but was overestimated, feature mainly attributed overstated isoprene. potential consequences overestimation inhibiting from modeling system. Results indicated BSOA generally increased base-case simulation enabled emissions. latest shift reactions compounds radicals, further suggested reduction α-pinene concentrations. Finally, briefly analyze differences Cloud Liquid Water Content (clwc) among Model’s clwc values SMEAR-II site, higher loads, likely numbered particles capable activating cloud droplets.

Language: Английский

Olfaction in the Anthropocene: NO 3 negatively affects floral scent and nocturnal pollination DOI
J. K. Chan, Sriram Parasurama, R. Atlas

et al.

Science, Journal Year: 2024, Volume and Issue: 383(6683), P. 607 - 611

Published: Feb. 8, 2024

There is growing concern about sensory pollutants affecting ecological communities. Anthropogenically enhanced oxidants [ozone (O 3 ) and nitrate radicals (NO )] rapidly degrade floral scents, potentially reducing pollinator attraction to flowers. However, the physiological behavioral impacts on pollinators plant fitness are unknown. Using a nocturnal flower-moth system, we found that atmospherically relevant concentrations of NO eliminate flower visitation by moths, reaction with subset monoterpenes what reduces scent’s attractiveness. Global atmospheric models scent oxidation reveal in certain urban areas may have reduced ability perceive navigate These results illustrate impact anthropogenic an animal’s olfactory indicate such be critical regulators global pollination.

Language: Английский

Citations

10
Formation of highly oxygenated organic molecules from the oxidation of limonene by OH radical: significant contribution of H-abstraction pathway DOI Creative Commons
Hao Luo, Luc Vereecken, Hongru Shen

et al.

Atmospheric chemistry and physics, Journal Year: 2023, Volume and Issue: 23(13), P. 7297 - 7319

Published: July 4, 2023

Abstract. Highly oxygenated organic molecules (HOMs) play a pivotal role in the formation of secondary aerosol (SOA). Therefore, distribution and yields HOMs are fundamental to understand their fate chemical evolution atmosphere, it is conducive ultimately assess impact SOA on air quality climate change. In this study, gas-phase formed from reaction limonene with OH radicals photooxidation were investigated SAPHIR (Simulation Atmospheric PHotochemistry large Reaction chamber), using time-of-flight ionization mass spectrometer nitrate reagent ion (NO3--CIMS). A number HOMs, including monomers (C9–10) dimers (C17–20), detected classified into various families. Both closed-shell products open-shell peroxy (RO2) identified under low NO (0.06–0.1 ppb) high conditions (17 ppb). C10 most abundant HOM account for over 80 % total HOMs. Closed-shell two radical family, C10H15Ox⚫ (x=6–15) C10H17Ox⚫ (x=6–15), respective termination reactions NO, RO2, HO2. While likely by addition C10H16, dominant initial step plus OH, C10H15Ox⚫, via H abstraction OH. related contributed 41 42 at demonstrating that H-abstraction pathways significant Combining theoretical kinetic calculations, structure–activity relationships (SARs), data literature, observed RO2 intensities, we proposed tentative mechanisms both pathways. We further estimated molar be 1.97-1.06+2.52 0.29-0.16+0.38 respectively. Our study highlights importance provides yield oxidation simulate formation.

Language: Английский

Citations

14
Modeling Secondary Organic Aerosols in China: State of the Art and Perspectives DOI
Jingyi Li, Haowen Zhang, Lin Li

et al.

Current Pollution Reports, Journal Year: 2023, Volume and Issue: unknown

Published: Jan. 16, 2023

Language: Английский

Citations

12
On the formation of biogenic secondary organic aerosol in chemical transport models: an evaluation of the WRF-CHIMERE (v2020r2) model with a focus over the Finnish boreal forest DOI Creative Commons
Giancarlo Ciarelli,

Sara Tahvonen,

Arineh Cholakian

et al.

Geoscientific model development, Journal Year: 2024, Volume and Issue: 17(2), P. 545 - 565

Published: Jan. 24, 2024

Abstract. We present an evaluation of the regional chemical transport model (CTM) WRF-CHIMERE (v2020r2) for formation biogenic secondary organic aerosol (BSOA) with a focus over Finnish boreal forest. Formation processes aerosols are still affected by different sources uncertainties, and predictions vary greatly depending on levels details adopted emissions schemes. In this study, air quality simulations were conducted summer 2019 using (OA) schemes (as currently available in literature) to treat BSOA. First, we performed set framework volatility basis (VBS) scheme carrying assumptions treatment aging The results compared against high-resolution (i.e., 1 h) mass size distribution measurements at Station Measuring Ecosystem–Atmosphere Relations (SMEAR-II) site located Hyytiälä, addition other gas-phase species such as ozone (O3), nitrogen oxides (NOx), volatile compound (BVOC) isoprene (C5H10) monoterpenes. show that could reproduce well diurnal variation measured OA concentrations all investigated scenarios (along standard meteorological parameters) increase during specific heat wave episodes. However, modeled varied between used describe BSOA, also confirmed additional carbon (OC) measurement data retrieved from EBAS European databases. Comparisons monoterpene revealed captured observed concentrations, but was largely overestimated, feature mainly attributed overstated isoprene. potential consequences overestimation inhibiting modeling system. Results indicated BSOA increased northern regions domain (e.g., Finland) southern countries, possibly due shift reactions compounds radicals, further suggested reduction α-pinene concentrations. Finally, briefly analyze differences cloud liquid water content (clwc) among clwc values SMEAR-II site, higher loads, most likely result number particles capable activating droplets.

Language: Английский

Citations

4
Interactions of peroxy radicals from monoterpene and isoprene oxidation simulated in the radical volatility basis set DOI Creative Commons
Meredith Schervish, Martin Heinritzi, Dominik Stolzenburg

et al.

Environmental Science Atmospheres, Journal Year: 2024, Volume and Issue: 4(7), P. 740 - 753

Published: Jan. 1, 2024

Isoprene affects new particle formation rates in environments and experiments also containing monoterpenes.

Language: Английский

Citations

4
Kinetic Modeling of Secondary Organic Aerosol in a Weather-Chemistry Model: Parameterizations, Processes, and Predictions for GOAmazon DOI
Yicong He, Kelsey R. Bilsback, Manish Shrivastava

et al.

ACS ES&T Air, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 24, 2025

Language: Английский

Citations

0
Global Simulations of Phase State and Equilibration Time Scales of Secondary Organic Aerosols with GEOS-Chem DOI Creative Commons

R. Phan Tan Luu,

Meredith Schervish, Nicole A. June

et al.

ACS Earth and Space Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 10, 2025

The phase state of secondary organic aerosols (SOA) can range from liquid through amorphous semisolid to glassy solid, which is important consider as it influences various multiphase processes including SOA formation and partitioning, chemistry, cloud activation. In this study, we simulate the glass transition temperature viscosity over globe using global chemical transport model, GEOS-Chem. simulated spatial distributions show that at surface exist equatorial regions oceans, in midlatitude continental regions, solid lands with low relative humidity. predicted viscosities are mostly consistent available measurements. free troposphere, particles be 850 hPa 500 hPa, except tropical Amazonia, where viscous. Phase also exhibits seasonal variation a higher frequency winter compared warmer seasons. We calculate equilibration time scales partitioning (τeq) effective mass accommodation coefficient (αeff), indicating τeq shorter than step GEOS-Chem 20 min αeff close unity for most locations level, supporting application equilibrium partitioning. However, prolonged lowered drylands upper suggesting kinetically limited growth would need considered these future large-scale model studies.

Language: Английский

Citations

0
High frequency of new particle formation events driven by summer monsoon in the central Tibetan Plateau, China DOI Creative Commons
Lizi Tang, Min Hu, Dongjie Shang

et al.

Atmospheric chemistry and physics, Journal Year: 2023, Volume and Issue: 23(7), P. 4343 - 4359

Published: April 13, 2023

Abstract. New particle formation (NPF) is an important source of cloud condensation nuclei (CCN), which affects Earth's radiative balance and global climate. The mechanism CCN contribution NPF at the high-altitude mountains, especially in Tibetan Plateau (TP), was unclear due to lack measurements. In this study, intensive measurements were conducted Nam Co station (4730 m a.s.l.) central TP during both pre-monsoon summer monsoon seasons. frequencies events exhibited evident seasonal differences with 15 % season 80 season. comprehensive analysis measured sink (CS), gaseous precursors meteorological conditions, supplemented by model simulations SO2 volatile organic compound (VOC), points involved nucleation as dominant mechanism. Condensation sulfuric acid could have no significant effect on occurrence events. frequent may result from higher frequency southerly southwesterly air masses, brought participate process. It had increased aerosol number concentrations supersaturation 1.2 more than 2 0.6 times compared those season, respectively. Considering that smaller particles formed further grow reach size following days low-level coagulation sink, amount potential be much larger our local measurement results. Our results emphasized importance considering when simulating amounts aerosols atmosphere. Long-term investigations a full set instrumentation are required for deeper scientific understanding process its role budget TP.

Language: Английский

Citations

6
Photooxidation-Initiated Aqueous-Phase Formation of Organic Peroxides: Delving into Formation Mechanisms DOI
Tania Gautam,

Erica Kim,

L.‐K. Ng

et al.

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(15), P. 6564 - 6574

Published: April 5, 2024

Formation of highly oxygenated molecules (HOMs) such as organic peroxides (ROOR, ROOH, and H2O2) is known to degrade food matter. Gas-phase unimolecular autoxidation bimolecular RO2 + HO2/RO2 reactions are prominently renowned mechanisms associated with the formation peroxides. However, reaction pathways conditions favoring generation in aqueous phase need be evaluated. Here, we identified bulk aqueous-phase ROOHs varying precursors, including a laboratory model compound monoterpene oxidation products. Our results show that suppressed at enhanced oxidant concentrations but exhibits complex trends elevated precursor concentrations. Furthermore, observed an exponential increase yield when UV light longer wavelengths was used experiment, comparing UVA, UVB, UVC. Water-soluble compounds represent significant fraction ambient cloud-water components (up 500 μM). Thus, facilitating HOMs (i.e., ROOHs) during water-soluble species add climate health burden atmospheric particulate

Language: Английский

Citations

1
Ring-opening yields and auto-oxidation rates of the resulting peroxy radicals from OH-oxidation of α-pinene and β-pinene DOI Creative Commons
Ben H. Lee, Siddharth Iyer, Theo Kurtén

et al.

Environmental Science Atmospheres, Journal Year: 2023, Volume and Issue: 3(2), P. 399 - 407

Published: Jan. 1, 2023

Atmospheric oxidation of monoterpenes (C 10 H 16 ) contributes to ambient particle number and mass concentrations due, in part, the resulting peroxy radicals undergoing auto-oxidation low-volatility highly oxygenated molecules (HOMs).

Language: Английский

Citations

3