DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Solid organic-coated ammonium sulfate particles at high relative humidity in the summertime Arctic atmosphere

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
ORCiD logo [1];  [1];  [2]; ORCiD logo [1];  [1];  [3];  [3]; ORCiD logo [4];  [4];  [5]; ORCiD logo [6]; ORCiD logo [7];  [2]; ORCiD logo [6];  [3]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of Michigan, Ann Arbor, MI (United States)
  2. Univ. of the Pacific, Stockton, CA (United States)
  3. Baylor Univ., Waco, TX (United States)
  4. Univ. of Washington, Seattle, WA (United States)
  5. Univ. of Washington, Seattle, WA (United States); National Oceanic and Atmospheric Administration (NOAA), Seattle, WA (United States). Pacific Marine Environmental Laboratory
  6. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
  7. National Oceanic and Atmospheric Administration (NOAA), Seattle, WA (United States). Pacific Marine Environmental Laboratory

The ability of atmospheric aerosols to impact climate through water uptake and cloud formation is fundamentally determined by the size, composition, and phase (liquid, semisolid, or solid) of individual particles. Particle phase is dependent on atmospheric conditions (relative humidity and temperature) and chemical composition and, importantly, solid particles can inhibit the uptake of water and other trace gases, even under humid conditions. Particles composed primarily of ammonium sulfate are presumed to be liquid at the relative humidities (67 to 98%) and temperatures (–2 to 4 °C) of the summertime Arctic. Under these atmospheric conditions, we report the observation of solid organic-coated ammonium sulfate particles representing 30% of particles, by number, in a key size range (<0.2 µm) for cloud activation within marine air masses from the Arctic Ocean at Utqiagvik, AK. The composition and size of the observed particles are consistent with recent Arctic modeling and observational results showing new particle formation and growth from dimethylsulfide oxidation to form sulfuric acid, reaction with ammonia, and condensation of marine biogenic sulfate and highly oxygenated organic molecules. Aqueous sulfate particles typically undergo efflorescence and solidify at relative humidities of less than 34%. Therefore, the observed solid phase is hypothesized to occur from contact efflorescence during collision of a newly formed Aitken mode sulfate particle with an organic-coated ammonium sulfate particle. With declining sea ice in the warming Arctic, this particle source is expected to increase with increasing open water and marine biogenic emissions.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center; Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL); University of Michigan, Ann Arbor, MI (United States)
Sponsoring Organization:
National Oceanic and Atmospheric Administration (NOAA); National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Biological and Environmental Research (BER)
Contributing Organization:
Argonne National Laboratory (ANL); Brookhaven National Laboratory (BNL); Oak Ridge National Laboratory (ORNL); Pacific Northwest National Laboratory (PNNL)
Grant/Contract Number:
AC05-76RL01830; AC06-76RL01830; SC0019172
OSTI ID:
1857331
Report Number(s):
DOE-UMICH--SC0019172; PNNL-SA-160900
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 14 Vol. 119; ISSN 0027-8424
Publisher:
National Academy of SciencesCopyright Statement
Country of Publication:
United States
Language:
English

References (54)

Indirect evidence of the composition of nucleation mode atmospheric particles in the high Arctic: COMPOSITION OF NUCLEATION ARCTIC AEROSOL journal January 2016
Phase imaging as an extension to tapping mode AFM for the identification of material properties on humidity-sensitive surfaces journal June 1997
Processes and impacts of Arctic amplification: A research synthesis journal May 2011
Automated Chemical Analysis of Internally Mixed Aerosol Particles Using X-ray Spectromicroscopy at the Carbon K-Edge journal October 2010
Cryo-Transmission Electron Microscopy Imaging of the Morphology of Submicrometer Aerosol Containing Organic Acids and Ammonium Sulfate journal February 2014
Liquid–Liquid Phase Separation in Supermicrometer and Submicrometer Aerosol Particles journal May 2020
Atomic Force Microscopy-Infrared Spectroscopy of Individual Atmospheric Aerosol Particles: Subdiffraction Limit Vibrational Spectroscopy and Morphological Analysis journal August 2017
Solid, Semisolid, and Liquid Phase States of Individual Submicrometer Particles Directly Probed Using Atomic Force Microscopy journal November 2017
Particle-Phase Diffusion Modulates Partitioning of Semivolatile Organic Compounds to Aged Secondary Organic Aerosol journal January 2020
Effect of the Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive Uptake of Isoprene-Derived Epoxydiols (IEPOX) journal February 2018
Seeded Crystal Growth of Internally Mixed Organic–Inorganic Aerosols: Impact of Organic Phase State journal September 2021
Biological Impacts on Carbon Speciation and Morphology of Sea Spray Aerosol journal October 2017
Optical Property Measurements and Single Particle Analysis of Secondary Organic Aerosol Produced from the Aqueous-Phase Reaction of Ammonium Sulfate with Methylglyoxal journal February 2018
Reactive Uptake of Isoprene Epoxydiols Increases the Viscosity of the Core of Phase-Separated Aerosol Particles journal May 2019
Atmospheric Processes and Their Controlling Influence on Cloud Condensation Nuclei Activity journal February 2015
Investigation of Surface Changes of Nanoparticles Using TM-AFM Phase Imaging journal May 2003
Surface Organic Monolayers Control the Hygroscopic Growth of Submicrometer Particles at High Relative Humidity journal May 2014
Solid/Liquid Phase Diagram of the Ammonium Sulfate/Succinic Acid/Water System journal December 2014
Ammonium Sulfate:  Equilibrium and Metastability Phase Diagrams from 40 to −50 °C journal September 1998
Deliquescence, efflorescence, and supercooling of ammonium sulfate aerosols at low temperature: Implications for cirrus cloud formation and aerosol phase in the atmosphere journal June 1999
Infrared spectroscopic study of the deliquescence and efflorescence of ammonium sulfate aerosol as a function of temperature journal September 1999
Deliquescence behavior of organic/ammonium sulfate aerosol: DELIQUESCENCE BEHAVIOR OF ORGANIC/AMMONIUM SULFATE AEROSOL journal October 2002
Chemical speciation of sulfur in marine cloud droplets and particles: Analysis of individual particles from the marine boundary layer over the California current journal January 2008
Aerosol Mixing State: Measurements, Modeling, and Impacts journal May 2019
The Seasonal and Regional Transition to an Ice‐Free Arctic journal January 2021
Differing Mechanisms of New Particle Formation at Two Arctic Sites journal February 2021
Contribution of Arctic seabird-colony ammonia to atmospheric particles and cloud-albedo radiative effect journal November 2016
Global distribution of particle phase state in atmospheric secondary organic aerosols journal April 2017
Resilience of persistent Arctic mixed-phase clouds journal December 2011
Airborne soil organic particles generated by precipitation journal May 2016
Small fraction of marine cloud condensation nuclei made up of sea spray aerosol journal August 2017
The viscosity of atmospherically relevant organic particles journal March 2018
Atomic number dependence of Z contrast in scanning transmission electron microscopy journal August 2018
Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere journal January 2011
In-situ measurements of the mixing state and optical properties of soot with implications for radiative forcing estimates journal July 2009
Viscosity of  -pinene secondary organic material and implications for particle growth and reactivity journal April 2013
Contact efflorescence as a pathway for crystallization of atmospherically relevant particles journal December 2015
Microlayer source of oxygenated volatile organic compounds in the summertime marine Arctic boundary layer journal May 2017
Multiphase reactivity of polycyclic aromatic hydrocarbons is driven by phase separation and diffusion limitations journal May 2019
Solid Ammonium Sulfate Aerosols as Ice Nuclei: A Pathway for Cirrus Cloud Formation journal September 2006
Getting to the Critical Nucleus of Aerosol Formation journal June 2010
Polysaccharides, Proteins, and Phytoplankton Fragments: Four Chemically Distinct Types of Marine Primary Organic Aerosol Classified by Single Particle Spectromicroscopy journal January 2010
AFM–IR: Combining Atomic Force Microscopy and Infrared Spectroscopy for Nanoscale Chemical Characterization journal December 2012
Variability of humidity conditions in the Arctic during the first International Polar Year, 1882–83 journal January 2014
Depositional ice nucleation on solid ammonium sulfate and glutaric acid particles journal January 2010
Heterogeneous ice nucleation on phase-separated organic-sulfate particles: effect of liquid vs. glassy coatings journal January 2013
Competition between water uptake and ice nucleation by glassy organic aerosol particles journal January 2014
Hygroscopic and phase separation properties of ammonium sulfate/organics/water ternary solutions journal January 2015
Processes controlling the annual cycle of Arctic aerosol number and size distributions journal January 2016
Contributions of transported Prudhoe Bay oil field emissions to the aerosol population in Utqiaġvik, Alaska journal January 2017
Organic coating on sulfate and soot particles during late summer in the Svalbard Archipelago journal January 2019
Dimethyl sulfide and its role in aerosol formation and growth in the Arctic summer – a modelling study journal January 2019
The effect of hydrophobic glassy organic material on the cloud condensation nuclei activity of particles with different morphologies journal January 2019
Characterization of aerosol growth events over Ellesmere Island during the summers of 2015 and 2016 journal January 2019