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Title: Long-term variability in immersion-mode marine ice-nucleating particles from climate model simulations and observations

Abstract

Ice-nucleating particles (INPs) in the Southern Ocean (SO) atmosphere have significant impacts on cloud radiative and microphysical properties. Yet, INP prediction skill in climate models remains poorly understood, in part because of the lack of long-term measurements. Here we show, for the first time, how model-simulated INP concentrations compare with year-round INP measurements during the Macquarie Island Cloud Radiation Experiment (MICRE) campaign from 2017–2018. We simulate immersion-mode INP concentrations using the Energy Exascale Earth System Model version 1 (E3SMv1) by combining simulated aerosols with recently developed deterministic INP parameterizations and the native classical nucleation theory (CNT) for mineral dust in E3SMv1. Because MICRE did not collect aerosol measurements of super-micron particles, which are more effective ice nucleators, we evaluate the model's aerosol fields at other high-latitude sites using long-term in situ observations of dust and sea spray aerosol. We find that the model underestimates dust and overestimates sea spray aerosol concentrations by 1 to 2 orders of magnitude for most of the high-latitude sites in the Southern Hemisphere. We next compare predicted INP concentrations with concentrations of INPs collected on filter samples (typically for 2 or 3 d) and processed offline using the Colorado State University ice spectrometer (IS) inmore » immersion freezing mode. We find that when deterministic parameterizations for both dust and sea spray INPs are used, simulated INPs are within a factor of 10 of observed INPs more than 60 % of the time during summer. Our results also indicate that the E3SM's current treatment of mineral dust immersion freezing in the SO is impacted by compensating biases – an underprediction of dust amount was compensated by an overprediction of its effectiveness as INPs. We also perform idealized droplet freezing experiments to quantify the implications of the time-dependent behavior assumed by the E3SM's CNT-parameterization and compare with the ice spectrometer observations. We find that the E3SM CNT 10 s diagnostic used in this study is a reasonable approximation of the exact formulation of CNT, when applied to ice spectrometer measurements in low-INP conditions similar to Macquarie Island. However, the linearized 10 s diagnostic underestimates the exact formula by an order of magnitude or more in places with high-INP conditions like the Sahara. Overall, our findings suggest that it is important to correct the biases in E3SM's simulated dust life cycle and update E3SM's INP parameterizations. INP prediction errors of 2 to 3 orders of magnitude can have considerable impacts on the simulated cloud and radiative properties in global climate models. On comparing INP concentrations during MICRE against ship-based campaigns, Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS) and Antarctic Circumnavigation Expedition (ACE), we find that INPs from the latter are significantly higher only in regions closer to Macquarie Island. This alludes to the fact that physical, chemical and biological processes affecting INP concentrations as stimulated by the island could be partly responsible for the high INP concentrations observed at Macquarie Island during the MICRE campaign. Therefore, improvements to both aerosol simulation and INP parameterizations are required to adequately simulate INPs and their cloud impacts in E3SM. It will be helpful to include a parallel measurement of the size-resolved aerosol composition and explore opportunities for long-term measurement platforms in future field campaigns studying INP sources in remote marine regions.« less

Authors:
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Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center; Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
Contributing Org.:
Pacific Northwest National Laboratory (PNNL); Brookhaven National Laboratory (BNL); Argonne National Laboratory (ANL)
OSTI Identifier:
1974813
Alternate Identifier(s):
OSTI ID: 1985656; OSTI ID: 1985982
Report Number(s):
PNNL-SA-171035
Journal ID: ISSN 1680-7324
Grant/Contract Number:  
KP1701010/72149; 65814; AC05-76RL01830; SC0021116; AC02-05CH11231
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 23 Journal Issue: 10; Journal ID: ISSN 1680-7324
Publisher:
Copernicus GmbH
Country of Publication:
Germany
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Raman, Aishwarya, Hill, Thomas, DeMott, Paul J., Singh, Balwinder, Zhang, Kai, Ma, Po-Lun, Wu, Mingxuan, Wang, Hailong, Alexander, Simon P., and Burrows, Susannah M. Long-term variability in immersion-mode marine ice-nucleating particles from climate model simulations and observations. Germany: N. p., 2023. Web. doi:10.5194/acp-23-5735-2023.
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Raman, Aishwarya, Hill, Thomas, DeMott, Paul J., Singh, Balwinder, Zhang, Kai, Ma, Po-Lun, Wu, Mingxuan, Wang, Hailong, Alexander, Simon P., & Burrows, Susannah M. Long-term variability in immersion-mode marine ice-nucleating particles from climate model simulations and observations. Germany. https://doi.org/10.5194/acp-23-5735-2023
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Raman, Aishwarya, Hill, Thomas, DeMott, Paul J., Singh, Balwinder, Zhang, Kai, Ma, Po-Lun, Wu, Mingxuan, Wang, Hailong, Alexander, Simon P., and Burrows, Susannah M. Tue . "Long-term variability in immersion-mode marine ice-nucleating particles from climate model simulations and observations". Germany. https://doi.org/10.5194/acp-23-5735-2023.
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@article{osti_1974813,
title = {Long-term variability in immersion-mode marine ice-nucleating particles from climate model simulations and observations},
author = {Raman, Aishwarya and Hill, Thomas and DeMott, Paul J. and Singh, Balwinder and Zhang, Kai and Ma, Po-Lun and Wu, Mingxuan and Wang, Hailong and Alexander, Simon P. and Burrows, Susannah M.},
abstractNote = {Ice-nucleating particles (INPs) in the Southern Ocean (SO) atmosphere have significant impacts on cloud radiative and microphysical properties. Yet, INP prediction skill in climate models remains poorly understood, in part because of the lack of long-term measurements. Here we show, for the first time, how model-simulated INP concentrations compare with year-round INP measurements during the Macquarie Island Cloud Radiation Experiment (MICRE) campaign from 2017–2018. We simulate immersion-mode INP concentrations using the Energy Exascale Earth System Model version 1 (E3SMv1) by combining simulated aerosols with recently developed deterministic INP parameterizations and the native classical nucleation theory (CNT) for mineral dust in E3SMv1. Because MICRE did not collect aerosol measurements of super-micron particles, which are more effective ice nucleators, we evaluate the model's aerosol fields at other high-latitude sites using long-term in situ observations of dust and sea spray aerosol. We find that the model underestimates dust and overestimates sea spray aerosol concentrations by 1 to 2 orders of magnitude for most of the high-latitude sites in the Southern Hemisphere. We next compare predicted INP concentrations with concentrations of INPs collected on filter samples (typically for 2 or 3 d) and processed offline using the Colorado State University ice spectrometer (IS) in immersion freezing mode. We find that when deterministic parameterizations for both dust and sea spray INPs are used, simulated INPs are within a factor of 10 of observed INPs more than 60 % of the time during summer. Our results also indicate that the E3SM's current treatment of mineral dust immersion freezing in the SO is impacted by compensating biases – an underprediction of dust amount was compensated by an overprediction of its effectiveness as INPs. We also perform idealized droplet freezing experiments to quantify the implications of the time-dependent behavior assumed by the E3SM's CNT-parameterization and compare with the ice spectrometer observations. We find that the E3SM CNT 10 s diagnostic used in this study is a reasonable approximation of the exact formulation of CNT, when applied to ice spectrometer measurements in low-INP conditions similar to Macquarie Island. However, the linearized 10 s diagnostic underestimates the exact formula by an order of magnitude or more in places with high-INP conditions like the Sahara. Overall, our findings suggest that it is important to correct the biases in E3SM's simulated dust life cycle and update E3SM's INP parameterizations. INP prediction errors of 2 to 3 orders of magnitude can have considerable impacts on the simulated cloud and radiative properties in global climate models. On comparing INP concentrations during MICRE against ship-based campaigns, Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS) and Antarctic Circumnavigation Expedition (ACE), we find that INPs from the latter are significantly higher only in regions closer to Macquarie Island. This alludes to the fact that physical, chemical and biological processes affecting INP concentrations as stimulated by the island could be partly responsible for the high INP concentrations observed at Macquarie Island during the MICRE campaign. Therefore, improvements to both aerosol simulation and INP parameterizations are required to adequately simulate INPs and their cloud impacts in E3SM. It will be helpful to include a parallel measurement of the size-resolved aerosol composition and explore opportunities for long-term measurement platforms in future field campaigns studying INP sources in remote marine regions.},
doi = {10.5194/acp-23-5735-2023},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 10,
volume = 23,
place = {Germany},
year = {Tue May 23 00:00:00 EDT 2023},
month = {Tue May 23 00:00:00 EDT 2023}
}
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  • DOI: 10.1029/2020EF001673

Occurrence, liquid water content, and fraction of supercooled water clouds from combined CALIOP/IIR/MODIS measurements
journal, January 2010

  • Hu, Yongxiang; Rodier, Sharon; Xu, Kuan-man
  • Journal of Geophysical Research, Vol. 115
  • DOI: 10.1029/2009JD012384

New type of evidence for secondary ice formation at around −15 °C in mixed-phase clouds
journal, January 2019

  • Mignani, Claudia; Creamean, Jessie M.; Zimmermann, Lukas
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 2
  • DOI: 10.5194/acp-19-877-2019

Nucleation Processes in Deep Convection Simulated by a Cloud-System-Resolving Model with Double-Moment Bulk Microphysics
journal, March 2007

  • Phillips, Vaughan T. J.; Donner, Leo J.; Garner, Stephen T.
  • Journal of the Atmospheric Sciences, Vol. 64, Issue 3
  • DOI: 10.1175/JAS3869.1

On the evaluation of global sea-salt aerosol models at coastal/orographic sites
journal, January 2015

Aerosols at the poles: an AeroCom Phase II multi-model evaluation
journal, January 2017

  • Sand, Maria; Samset, Bjørn H.; Balkanski, Yves
  • Atmospheric Chemistry and Physics, Vol. 17, Issue 19
  • DOI: 10.5194/acp-17-12197-2017

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles
journal, January 2015

  • DeMott, P. J.; Prenni, A. J.; McMeeking, G. R.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 1
  • DOI: 10.5194/acp-15-393-2015

Characterization of aerosol properties at Cyprus, focusing on cloud condensation nuclei and ice-nucleating particles
journal, January 2019

  • Gong, Xianda; Wex, Heike; Müller, Thomas
  • Atmospheric Chemistry and Physics, Vol. 19, Issue 16
  • DOI: 10.5194/acp-19-10883-2019

Ship-based measurements of ice nuclei concentrations over the Arctic, Atlantic, Pacific and Southern oceans
journal, December 2020

  • Welti, André; Bigg, E. Keith; DeMott, Paul J.
  • Atmospheric Chemistry and Physics, Vol. 20, Issue 23
  • DOI: 10.5194/acp-20-15191-2020

Observational constraints on mixed-phase clouds imply higher climate sensitivity
journal, April 2016

A marine biogenic source of atmospheric ice-nucleating particles
journal, September 2015

  • Wilson, Theodore W.; Ladino, Luis A.; Alpert, Peter A.
  • Nature, Vol. 525, Issue 7568
  • DOI: 10.1038/nature14986

Effects of cloud condensation nuclei and ice nucleating particles on precipitation processes and supercooled liquid in mixed-phase orographic clouds
journal, January 2017

  • Fan, Jiwen; Leung, L. Ruby; Rosenfeld, Daniel
  • Atmospheric Chemistry and Physics, Vol. 17, Issue 2
  • DOI: 10.5194/acp-17-1017-2017

Do dust emissions from sparsely vegetated regions dominate atmospheric iron supply to the Southern Ocean?
journal, April 2017

  • Ito, Akinori; Kok, Jasper F.
  • Journal of Geophysical Research: Atmospheres, Vol. 122, Issue 7
  • DOI: 10.1002/2016JD025939

Intercomparison of the cloud water phase among global climate models: CLOUD WATER PHASE IN GCMs
journal, March 2014

  • Komurcu, Muge; Storelvmo, Trude; Tan, Ivy
  • Journal of Geophysical Research: Atmospheres, Vol. 119, Issue 6
  • DOI: 10.1002/2013JD021119

Black Carbon Particles Do Not Matter for Immersion Mode Ice Nucleation
journal, June 2020

  • Kanji, Zamin A.; Welti, André; Corbin, Joel C.
  • Geophysical Research Letters, Vol. 47, Issue 11
  • DOI: 10.1029/2019GL086764

Natural aerosols explain seasonal and spatial patterns of Southern Ocean cloud albedo
journal, July 2015

  • McCoy, Daniel T.; Burrows, Susannah M.; Wood, Robert
  • Science Advances, Vol. 1, Issue 6
  • DOI: 10.1126/sciadv.1500157

Importance of Supermicron Ice Nucleating Particles in Nascent Sea Spray
journal, February 2021

  • Mitts, Brock A.; Wang, Xiaofei; Lucero, Dolan D.
  • Geophysical Research Letters, Vol. 48, Issue 3
  • DOI: 10.1029/2020GL089633

Ice nuclei in marine air: biogenic particles or dust?
journal, January 2013

  • Burrows, S. M.; Hoose, C.; Pöschl, U.
  • Atmospheric Chemistry and Physics, Vol. 13, Issue 1
  • DOI: 10.5194/acp-13-245-2013

Simulating Observations of Southern Ocean Clouds and Implications for Climate
journal, October 2020

  • Gettelman, A.; Bardeen, C. G.; McCluskey, C. S.
  • Journal of Geophysical Research: Atmospheres, Vol. 125, Issue 21
  • DOI: 10.1029/2020JD032619

Laboratory simulations and parameterization of the primary marine aerosol production: THE PRIMARY MARINE AEROSOL SOURCE
journal, May 2003

  • Mårtensson, E. M.; Nilsson, E. D.; de Leeuw, G.
  • Journal of Geophysical Research: Atmospheres, Vol. 108, Issue D9
  • DOI: 10.1029/2002JD002263

Air mass characteristics, aerosol particle number concentrations, and number size distributions at Macquarie Island during the First Aerosol Characterization Experiment (ACE 1)
journal, July 1998

  • Brechtel, Fred J.; Kreidenweis, Sonia M.; Swan, Hilton B.
  • Journal of Geophysical Research: Atmospheres, Vol. 103, Issue D13
  • DOI: 10.1029/97JD03014

Sensitivity Study on the Influence of Cloud Microphysical Parameters on Mixed-Phase Cloud Thermodynamic Phase Partitioning in CAM5
journal, February 2016

Dust Radiative Effects on Climate by Glaciating Mixed‐Phase Clouds
journal, June 2019

  • Shi, Yang; Liu, Xiaohong
  • Geophysical Research Letters, Vol. 46, Issue 11
  • DOI: 10.1029/2019GL082504

An Overview of the Atmospheric Component of the Energy Exascale Earth System Model
journal, August 2019

  • Rasch, P. J.; Xie, S.; Ma, P. ‐L.
  • Journal of Advances in Modeling Earth Systems, Vol. 11, Issue 8
  • DOI: 10.1029/2019MS001629

Ice nucleation activity of agricultural soil dust aerosols from Mongolia, Argentina, and Germany: Ice Nucleation Activity of Soil Dust
journal, November 2016

  • Steinke, I.; Funk, R.; Busse, J.
  • Journal of Geophysical Research: Atmospheres, Vol. 121, Issue 22
  • DOI: 10.1002/2016JD025160

Satellite assessment of sea spray aerosol productivity: Southern Ocean case study
journal, January 2016

  • Witek, Marcin L.; Diner, David J.; Garay, Michael J.
  • Journal of Geophysical Research: Atmospheres, Vol. 121, Issue 2
  • DOI: 10.1002/2015JD023726

Representing a new MODIS consistent land surface in the Community Land Model (CLM 3.0)
journal, January 2007

  • Lawrence, Peter J.; Chase, Thomas N.
  • Journal of Geophysical Research, Vol. 112, Issue G1
  • DOI: 10.1029/2006JG000168

Secondary Ice Formation in Idealised Deep Convection—Source of Primary Ice and Impact on Glaciation
journal, May 2020

  • Miltenberger, Annette K.; Lüttmer, Tim; Siewert, Christoph
  • Atmosphere, Vol. 11, Issue 5
  • DOI: 10.3390/atmos11050542

Revisiting atmospheric dust export to the Southern Hemisphere ocean: Biogeochemical implications: DUST OVER THE SOUTHERN HEMISPHERE OCEAN
journal, April 2008

  • Wagener, Thibaut; Guieu, Cécile; Losno, Rémi
  • Global Biogeochemical Cycles, Vol. 22, Issue 2
  • DOI: 10.1029/2007GB002984

Agricultural harvesting emissions of ice-nucleating particles
journal, January 2018

  • Suski, Kaitlyn J.; Hill, Tom C. J.; Levin, Ezra J. T.
  • Atmospheric Chemistry and Physics, Vol. 18, Issue 18
  • DOI: 10.5194/acp-18-13755-2018

Chapter 7. Secondary Ice Production - current state of the science and recommendations for the future
journal, November 2016

Sea spray aerosol as a unique source of ice nucleating particles
journal, December 2015

  • DeMott, Paul J.; Hill, Thomas C. J.; McCluskey, Christina S.
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 21
  • DOI: 10.1073/pnas.1514034112

Stimulation of ice nucleation by marine diatoms
journal, December 2010

  • Knopf, D. A.; Alpert, P. A.; Wang, B.
  • Nature Geoscience, Vol. 4, Issue 2
  • DOI: 10.1038/ngeo1037

A Dynamic Link between Ice Nucleating Particles Released in Nascent Sea Spray Aerosol and Oceanic Biological Activity during Two Mesocosm Experiments
journal, January 2017

  • McCluskey, Christina S.; Hill, Thomas C. J.; Malfatti, Francesca
  • Journal of the Atmospheric Sciences, Vol. 74, Issue 1
  • DOI: 10.1175/JAS-D-16-0087.1

A new method to quantify mineral dust and other aerosol species from aircraft platforms using single-particle mass spectrometry
journal, January 2019

  • Froyd, Karl D.; Murphy, Daniel M.; Brock, Charles A.
  • Atmospheric Measurement Techniques, Vol. 12, Issue 11
  • DOI: 10.5194/amt-12-6209-2019

African dust deposition to Florida: Temporal and spatial variability and comparisons to models
journal, January 2010

  • Prospero, Joseph M.; Landing, William M.; Schulz, Michael
  • Journal of Geophysical Research, Vol. 115, Issue D13
  • DOI: 10.1029/2009JD012773

The temperature dependence of ice-nucleating particle concentrations affects the radiative properties of tropical convective cloud systems
journal, January 2021

  • Hawker, Rachel E.; Miltenberger, Annette K.; Wilkinson, Jonathan M.
  • Atmospheric Chemistry and Physics, Vol. 21, Issue 7
  • DOI: 10.5194/acp-21-5439-2021

Development of Heterogeneous Ice Nucleation Rate Coefficient Parameterizations From Ambient Measurements
journal, November 2021

  • Cornwell, Gavin C.; McCluskey, Christina S.; DeMott, Paul J.
  • Geophysical Research Letters, Vol. 48, Issue 23
  • DOI: 10.1029/2021GL095359

An improved hindcast approach for evaluation and diagnosis of physical processes in global climate models: AN IMPROVED HINDCAST APPROACH
journal, November 2015

  • Ma, H. -Y.; Chuang, C. C.; Klein, S. A.
  • Journal of Advances in Modeling Earth Systems, Vol. 7, Issue 4
  • DOI: 10.1002/2015MS000490

Biological aerosol particles as a key determinant of ice nuclei populations in a forest ecosystem: BIOLOGICAL ICE NUCLEI IN FOREST
journal, September 2013

  • Tobo, Yutaka; Prenni, Anthony J.; DeMott, Paul J.
  • Journal of Geophysical Research: Atmospheres, Vol. 118, Issue 17
  • DOI: 10.1002/jgrd.50801

Long-term measurements of the transport of African mineral dust to the southeastern United States: Implications for regional air quality
journal, July 1999

  • Prospero, Joseph M.
  • Journal of Geophysical Research: Atmospheres, Vol. 104, Issue D13
  • DOI: 10.1029/1999JD900072

Ice nucleation by fertile soil dusts: relative importance of mineral and biogenic components
journal, January 2014

  • O'Sullivan, D.; Murray, B. J.; Malkin, T. L.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 4
  • DOI: 10.5194/acp-14-1853-2014

Understanding processes that control dust spatial distributions with global climate models and satellite observations
journal, January 2020

  • Wu, Mingxuan; Liu, Xiaohong; Yu, Hongbin
  • Atmospheric Chemistry and Physics, Vol. 20, Issue 22
  • DOI: 10.5194/acp-20-13835-2020

Annual cycle observations of aerosols capable of ice formation in central Arctic clouds
journal, June 2022

The MACC-II 2007–2008 reanalysis: atmospheric dust evaluation and characterization over northern Africa and the Middle East
journal, January 2015

  • Cuevas, E.; Camino, C.; Benedetti, A.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 8
  • DOI: 10.5194/acp-15-3991-2015

High summertime aerosol organic functional group concentrations from marine and seabird sources at Ross Island, Antarctica, during AWARE
journal, January 2018

  • Liu, Jun; Dedrick, Jeramy; Russell, Lynn M.
  • Atmospheric Chemistry and Physics, Vol. 18, Issue 12
  • DOI: 10.5194/acp-18-8571-2018

Initiation of secondary ice production in clouds
journal, January 2018

  • Sullivan, Sylvia C.; Hoose, Corinna; Kiselev, Alexei
  • Atmospheric Chemistry and Physics, Vol. 18, Issue 3
  • DOI: 10.5194/acp-18-1593-2018

Spaceborne lidar observations of the ice-nucleating potential of dust, polluted dust, and smoke aerosols in mixed-phase clouds
journal, June 2014

  • Tan, Ivy; Storelvmo, Trude; Choi, Yong-Sang
  • Journal of Geophysical Research: Atmospheres, Vol. 119, Issue 11
  • DOI: 10.1002/2013JD021333

Contribution of feldspar and marine organic aerosols to global ice nucleating particle concentrations
journal, January 2017

  • Vergara-Temprado, Jesús; Murray, Benjamin J.; Wilson, Theodore W.
  • Atmospheric Chemistry and Physics, Vol. 17, Issue 5
  • DOI: 10.5194/acp-17-3637-2017

How important is biological ice nucleation in clouds on a global scale?
journal, April 2010

Change in atmospheric mineral aerosols in response to climate: Last glacial period, preindustrial, modern, and doubled carbon dioxide climates: DUST RESPONSE TO CLIMATE
journal, May 2006

  • Mahowald, Natalie M.; Muhs, Daniel R.; Levis, Samuel
  • Journal of Geophysical Research: Atmospheres, Vol. 111, Issue D10
  • DOI: 10.1029/2005JD006653

Immersion mode heterogeneous ice nucleation by an illite rich powder representative of atmospheric mineral dust
journal, January 2012

  • Broadley, S. L.; Murray, B. J.; Herbert, R. J.
  • Atmospheric Chemistry and Physics, Vol. 12, Issue 1
  • DOI: 10.5194/acp-12-287-2012

The distribution and biogeochemical importance of high-latitude dust in the Arctic and Southern Ocean-Antarctic regions: High-Latitude Dust
journal, March 2017

  • Bullard, Joanna E.
  • Journal of Geophysical Research: Atmospheres, Vol. 122, Issue 5
  • DOI: 10.1002/2016JD026363

Overview of Ice Nucleating Particles
journal, January 2017

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