Reply on AC1 DOI Creative Commons

Published: July 30, 2024

Abstract. Brown carbon (BrC) is a fraction of Organic Aerosols (OA) that absorbs radiation in the ultraviolet and short visible wavelengths. Its contribution to radiative forcing uncertain due limited knowledge its imaginary refractive index (k ). This study investigates variability k for OA from wildfires, residential, shipping, traffic emission sources over Europe. The MONARCH atmospheric chemistry model simulated concentrations source contributions, feeding an offline optical tool constrain values at 370 nm. was evaluated against mass Aerosol Chemical Speciation Monitors (ACSM) filter sample measurements, aerosol light absorption measurements nm derived AethalometerTM 12 sites across Results show captures temporal environments (regional, suburban urban background). Residential emissions are major colder months, while secondary organic aerosols (SOA) dominate warmer periods. Traffic minor primary contributor. Biomass coal combustion significantly influence absorption, with shipping also notable near harbors. Optimizing revealed significant influenced by environmental conditions. Derived biomass burning (0.03 0.13), residential (0.008 (0.005 0.08), 0.07) improved representation compared constant k. Introducing such source-specific constraints innovative approach enhance models.

Language: Английский

Fire Influence on Regional to Global Environments and Air Quality (FIREX‐AQ) DOI Creative Commons
C. Warneke, Joshua P. Schwarz, Jack E. Dibb

et al.

Journal of Geophysical Research Atmospheres, Journal Year: 2022, Volume and Issue: 128(2)

Published: Dec. 30, 2022

Abstract The NOAA/NASA Fire Influence on Regional to Global Environments and Air Quality (FIREX‐AQ) experiment was a multi‐agency, inter‐disciplinary research effort to: (a) obtain detailed measurements of trace gas aerosol emissions from wildfires prescribed fires using aircraft, satellites ground‐based instruments, (b) make extensive suborbital remote sensing fire dynamics, (c) assess local, regional, global modeling fires, (d) strengthen connections observables the ground such as fuels fuel consumption satellite products burned area radiative power. From Boise, ID western were studied with NASA DC‐8 two NOAA Twin Otter aircraft. high‐altitude ER‐2 deployed Palmdale, CA observe some these in conjunction overpasses other Further conducted three mobile laboratories sites, 17 different forecast analyses for fire, air quality climate implications. Salina, KS investigated 87 smaller Southeast in‐situ data collection. Sampling by all platforms designed measure gases aerosols multiple transects capture chemical transformation perform observations smoke plumes under day night conditions. linked consumed power orbital collected during overflights sampling fuels.

Language: Английский

Citations

82

Characteristics and evolution of brown carbon in western United States wildfires DOI Creative Commons
Linghan Zeng, Jack E. Dibb, E. Scheuer

et al.

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(12), P. 8009 - 8036

Published: June 21, 2022

Abstract. Brown carbon (BrC) associated with aerosol particles in western United States wildfires was measured between July and August 2019 aboard the NASA DC-8 research aircraft during Fire Influence on Regional to Global Environments Air Quality (FIREX-AQ) study. Two BrC measurement methods are investigated, highly spectrally resolved light absorption solvent (water methanol) extracts of collected filters situ bulk particle at three wavelengths (405, 532 664 nm) a photoacoustic spectrometer (PAS). A light-absorption closure analysis for 300 700 nm performed. The combined pure black material, including enhancements due internally mixed materials, plus soluble Mie-predicted factor conversion BrC, compared spectra from power law fit PAS wavelengths. For various parameters used, wavelength roughly 400 they agreed, lower individual component-predicted significantly exceeded higher consistently but more variable. Limitations extrapolation data below 405 missing species low solubility that strongly absorb may account differences. Based measurements closest fires, emission ratio PAS-measured relative monoxide (CO) average 0.13 Mm−1 ppbv−1; ratios also provided. As smoke moved away burning regions, evolution over time observed be complex; enhancement, depletion or constant levels age were all first 8 h after different plumes. Within following emissions, 4-nitrocatechol, well-characterized chromophore commonly found particles, largely depleted BrC. In descending plume where temperature increased by 15 K, 4-nitrocatechol dropped, possibly temperature-driven evaporation, remained unchanged. Evidence reactions ozone, related species, as pathway secondary formation under both high oxides nitrogen (NOx) conditions, while bleached regions ozone NOx, consistent complex behaviors laboratory studies. Although hours is variable, limited number aged (15 30 h) indicate net loss It yet determined how near-field affects characteristics longer timescales spatial scales, its environmental impacts likely greater.

Language: Английский

Citations

54

Characterization of brown carbon absorption in different European environments through source contribution analysis DOI Creative Commons
Héctor Navarro-Barboza, Jordi Rovira, Vincenzo Obiso

et al.

Atmospheric chemistry and physics, Journal Year: 2025, Volume and Issue: 25(4), P. 2667 - 2694

Published: Feb. 28, 2025

Abstract. Brown carbon (BrC) is a fraction of organic aerosol (OA) that absorbs radiation in the ultraviolet and short visible wavelengths. Its contribution to radiative forcing uncertain due limited knowledge its imaginary refractive index (k). This study investigates variability k for OA from wildfires, residential, shipping, traffic emission sources over Europe. The Multiscale Online Nonhydrostatic Atmosphere Chemistry (MONARCH) model simulated concentrations source contributions, feeding an offline optical tool constrain values at 370 nm. was evaluated against mass chemical speciation monitors (ACSMs) filter sample measurements, as well light absorption measurements nm derived Aethalometer™ 12 sites across Results show MONARCH captures temporal environments (regional, suburban, urban background). Residential emissions are major colder months, while secondary (SOA) dominates warmer periods. Traffic minor primary contributor. Biomass coal combustion significantly influence absorption, with shipping also notable near harbors. Optimizing revealed significant influenced by environmental conditions. Derived biomass burning (0.03 0.13), residential (0.008 (0.005 0.08), 0.07) improved representation compared constant k. Introducing such source-specific constraints innovative approach enhance atmospheric models.

Language: Английский

Citations

1

Reactive nitrogen and total organic carbon calibration techniques for the Aerodyne aerosol mass spectrometer DOI Creative Commons
Derek J. Price, Alison Piasecki, Rishabh U. Shah

et al.

Aerosol Science and Technology, Journal Year: 2023, Volume and Issue: 57(8), P. 727 - 741

Published: June 13, 2023

The Aerodyne aerosol mass spectrometer (AMS) is used extensively to measure the chemical composition of non-refractory submicron particles for laboratory and atmospheric field studies. Typical AMS calibration methods are mass-based, involving generating pure or mixtures with a known size number concentration. Here we present new method using heated platinum/molybdenum catalyst-based conversion technique that provides an independent measurement reactive nitrogen (Nr) total organic carbon (Cy) traceable gas-phase standards nitric oxide (NO) dioxide (CO2), respectively. was tested dried composed ammonium nitrate (AN), other salts, nitrogen-containing species. ionization efficiencies determined single particle Nr matched within experimental uncertainties (±15%). By measuring lens transmission efficiency incorporating light-scattering measurements collection efficiency, catalyst independently showed relative (RIE) essentially same among different containing compounds (±9%), regardless corresponding anion stoichiometry, quantifying support major assumption inherent in calibrations. Cy were calibrate RIE 4-nitrocatechol (1.1 ± 0.4), isosorbide mononitrate (1.2 0.1) triammonium citrate (2.1 0.2), which range RIEs quantitation. combined system provided more accurate elemental carbon-to-nitrogen ratios than high-resolution analysis Improved-Ambient plus inorganic nitrogen.

Language: Английский

Citations

12

Modeling atmospheric brown carbon in the GISS ModelE Earth system model DOI Creative Commons
Maegan A. DeLessio, Kostas Tsigaridis, Susanne E. Bauer

et al.

Atmospheric chemistry and physics, Journal Year: 2024, Volume and Issue: 24(10), P. 6275 - 6304

Published: May 29, 2024

Abstract. Brown carbon (BrC) is an absorbing organic aerosol (OA), primarily emitted through biomass burning (BB), which exhibits light absorption unique to both black (BC) and other aerosols. Despite many field laboratory studies seeking constrain BrC properties, the radiative forcing (RF) of still highly uncertain. To better understand its climate impact, we introduced One-Moment Aerosol (OMA) module GISS ModelE Earth system model (ESM). We assessed sensitivity primary processed a novel chemical aging scheme secondary formed from biogenic volatile compounds (BVOCs). Initial results show that typically contributes top-of-the-atmosphere (TOA) effect 0.04 W m−2. Sensitivity tests indicate explicitly simulating (separating it OAs), including BrC, bleaching contribute distinguishable effects should be accounted for in schemes. This addition prognostic allows greater physical complexity OA representation with no apparent trade-off performance, as evaluation optical depth against Robotic Network (AERONET) Moderate Resolution Imaging Spectroradiometer (MODIS) retrieval data, without scheme, reveals similar skill cases. Thus, simulated allow more physically based composition, crucial detailed like comparisons situ measurement campaigns. include summary best practices within at end this paper.

Language: Английский

Citations

4

Examination of brown carbon absorption from wildfires in the western US during the WE-CAN study DOI Creative Commons
Amy P. Sullivan, Rudra P. Pokhrel, Yingjie Shen

et al.

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(20), P. 13389 - 13406

Published: Oct. 18, 2022

Abstract. Light absorbing organic carbon, or brown carbon (BrC), can be a significant contributor to the visible light absorption budget. However, sources of BrC and contributions are not well understood. Biomass burning is thought major source BrC. Therefore, as part WE-CAN (Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption Nitrogen) study, data were collected on board National Science Foundation/National Center Atmospheric Research (NSF/NCAR) C-130 aircraft it intercepted smoke from wildfires in western US July–August 2018. measurements obtained near real-time using two techniques. The first coupled particle-into-liquid sampler (PILS) with liquid waveguide capillary cell total analyzer water-soluble WSOC (water-soluble carbon). second employed custom-built photoacoustic aerosol spectrometer (PAS) measure at 405 660 nm. PAS nm (PAS Abs BrC) was calculated by assuming determined equivalent black (BC) BC Ångström exponent 1. Data PILS combined investigate vs. various wildfire plumes sampled during WE-CAN. WSOC, 405, tracked each other out plumes. correlated (R2 value =0.42 =0.60) CO (carbon monoxide) =0.76 =0.55) all sampled. corrected non-water-soluble fraction UHSAS (ultra-high-sensitivity spectrometer) mass. showed good closure factor ∼1.5 2 difference. This difference explained particle bulk solution measured PILS, respectively, confirmed Mie theory calculations. During WE-CAN, ∼ 45 % (ranging 31 65 %) observed due species. ratio ΔCO no clear dependence fire dynamics time since emission over 9 h.

Language: Английский

Citations

18

Nitration of Phenols by Reaction with Aqueous Nitrite: A Pathway for the Formation of Atmospheric Brown Carbon DOI
Yutong Wang, Spiro Jorga, Jonathan P. D. Abbatt

et al.

ACS Earth and Space Chemistry, Journal Year: 2023, Volume and Issue: 7(3), P. 632 - 641

Published: Feb. 24, 2023

Nitrophenols are a major component of light-absorbing atmospheric organic aerosols, commonly referred to as brown carbon (BrC). Most nitrophenol formation pathways involve reactions phenolic compounds with OH, NO3, and NO2 in the gas phase. In this study, an aqueous production pathway is investigated that can proceed dark without apparent OH radical formation. Using high-performance liquid chromatography–mass spectrometry, we demonstrate catechol reacts acidic solutions dissolved nitrite form nitrocatechol. The rate nitration increases significantly from pH 4.4 3.4 such nitrocatechol susceptible second-generation under most conditions producing chromophores absorb visible region (peak at 425 nm). Increases N:C ratio reaction solution, detected by aerosol mass enhanced absorption 300 500 nm wood peat smoke extracts exposed suggest general pathway. which BrC process may occur discussed.

Language: Английский

Citations

10

Look Within: Intraplume Differences on Smoke Aerosol Aging Driven by Concentration Gradients DOI
Nicole A. June, Elizabeth B. Wiggins, Edward L. Winstead

et al.

Journal of Geophysical Research Atmospheres, Journal Year: 2025, Volume and Issue: 130(5)

Published: Feb. 26, 2025

Abstract The evolution of organic aerosol (OA) composition and size distributions within smoke plumes are uncertain due to variability in the rates OA evaporation/condensation coagulation a plume. It remains unclear how varies across different parts individual plumes. We use large eddy simulation model coupled with aerosol‐microphysics radiation models simulate Williams Flats fire sampled during Fire Influence on Regional Global Environments Air Quality field campaign. At aircraft altitude, captures observed changes through 4 hr aging. primary (POA), oxidized POA (OPOA), secondary (SOA) shows that >90% SOA formation occurs before first transect (∼40 min aging). Lidar observations show significant amount planetary boundary layer (PBL) free troposphere (FT) having equal amounts PBL FT. Due faster initial dilution, concentrations more than factor two lower FT concentrations, resulting slower coagulational growth PBL. A 20 K temperature decrease height influences evaporation near surface, while net is driven by continued dilution after transect. Net condensation result areas higher OH concentration leading OPOA formation. Our results motivate need for systematic vertical gradients

Language: Английский

Citations

0

Chemical Imaging of Atmospheric Biomass Burning Particles from North American Wildfires DOI
Felipe Rivera-Adorno, Jay M. Tomlin, Nurun Nahar Lata

et al.

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

Published: April 1, 2025

Language: Английский

Citations

0

Changes in Light Absorption and Chemical Properties for Biomass Burning Organic Aerosol over Long Time Scales DOI
Rachel E. O’Brien, Hongmin Yu, Natalie Warren

et al.

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

Published: April 7, 2025

Language: Английский

Citations

0