Articles | Volume 15, issue 24
https://doi.org/10.5194/acp-15-13819-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-15-13819-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Thermodynamic derivation of the activation energy for ice nucleation
NASA Goddard Space Flight Center, Greenbelt, MD, USA
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The Green's functions methodology offers a systematic, easy-to-implement, computationally cheap, scalable, and extendable method to tune uncertain parameters in models accounting for the dependent response of the model to a change in various parameters. Herein, we successfully show for the first time that long-term errors in earth system models can be considerably reduced using Green's functions methodology. The method can be easily applied to any model containing uncertain parameters.
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The study using the NASA Earth system model shows ~2.6 % increase in burning season gross primary production and ~1.5 % increase in annual net primary production across the Amazon Basin during 2010–2016 due to the change in surface downward direct and diffuse photosynthetically active radiation by biomass burning aerosols. Such an aerosol effect is strongly dependent on the presence of clouds. The cloud fraction at which aerosols switch from stimulating to inhibiting plant growth occurs at ~0.8.
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Increases in atmospheric aerosols affect the scattering and absorption of solar radiation by altering the macrophysical and microphysical processes of clouds. We analyzed aerosol–cloud interactions in response to degassing events from the Kilauea volcano in 2008 and 2018 by comparing satellite and simulated cloud properties. Results showed a threshold response to overcome meteorological effects that is largely controlled by aerosol concentration, composition, plume height, and ENSO state.
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This work provides a novel way of using polarized passive microwave measurements to study the interlinked cloud–convection–precipitation processes. The magnitude of differences between polarized radiances is found linked to ice microphysics (shape, size, orientation and density), mesoscale dynamic and thermodynamic structures, and surface precipitation. We conclude that passive sensors with multiple polarized channel pairs may serve as cheaper and useful substitutes for spaceborne radar sensors.
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This work develops a model for ice formation mediated by particles immersed within droplets. Ice nucleation is not only enhanced by the modification of the thermodynamic properties of the vicinal water but is also inhibited by decreased water mobility near the particle. The ice nucleation rate is thus determined by competing kinetic and thermodynamic factors during ice formation. A new regime where ice nucleation is mediated mainly by kinetics instead of thermodynamics is discovered.
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
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Y. C. Sud, D. Lee, L. Oreopoulos, D. Barahona, A. Nenes, and M. J. Suarez
Geosci. Model Dev., 6, 57–79, https://doi.org/10.5194/gmd-6-57-2013, https://doi.org/10.5194/gmd-6-57-2013, 2013
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Katherine H. Breen, Donifan Barahona, Tianle Yuan, Huisheng Bian, and Scott C. James
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Increases in atmospheric aerosols affect the scattering and absorption of solar radiation by altering the macrophysical and microphysical processes of clouds. We analyzed aerosol–cloud interactions in response to degassing events from the Kilauea volcano in 2008 and 2018 by comparing satellite and simulated cloud properties. Results showed a threshold response to overcome meteorological effects that is largely controlled by aerosol concentration, composition, plume height, and ENSO state.
Jie Gong, Xiping Zeng, Dong L. Wu, S. Joseph Munchak, Xiaowen Li, Stefan Kneifel, Davide Ori, Liang Liao, and Donifan Barahona
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This work develops a model for ice formation mediated by particles immersed within droplets. Ice nucleation is not only enhanced by the modification of the thermodynamic properties of the vicinal water but is also inhibited by decreased water mobility near the particle. The ice nucleation rate is thus determined by competing kinetic and thermodynamic factors during ice formation. A new regime where ice nucleation is mediated mainly by kinetics instead of thermodynamics is discovered.
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041, https://doi.org/10.5194/gmd-11-4021-2018, https://doi.org/10.5194/gmd-11-4021-2018, 2018
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The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
Sylvia C. Sullivan, Ricardo Morales Betancourt, Donifan Barahona, and Athanasios Nenes
Atmos. Chem. Phys., 16, 2611–2629, https://doi.org/10.5194/acp-16-2611-2016, https://doi.org/10.5194/acp-16-2611-2016, 2016
Short summary
Short summary
We use the adjoint model of a cirrus parameterization to quantify sources of crystal variability for various ice-nucleating spectra and output from CAM5.
The sensitivities can be directly linked to nucleation regime and
efficiency of various INP.
The lab-based spectrum calculates much higher INP efficiencies than field-based ones, owing to aerosol surface properties.
The sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters.
D. Barahona, A. Molod, J. Bacmeister, A. Nenes, A. Gettelman, H. Morrison, V. Phillips, and A. Eichmann
Geosci. Model Dev., 7, 1733–1766, https://doi.org/10.5194/gmd-7-1733-2014, https://doi.org/10.5194/gmd-7-1733-2014, 2014
D. Barahona
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Y. C. Sud, D. Lee, L. Oreopoulos, D. Barahona, A. Nenes, and M. J. Suarez
Geosci. Model Dev., 6, 57–79, https://doi.org/10.5194/gmd-6-57-2013, https://doi.org/10.5194/gmd-6-57-2013, 2013
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Subject: Clouds and Precipitation | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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Leslie Nuñez López, Pierre Amato, and Barbara Ervens
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Aishwarya Raman, Thomas Hill, Paul J. DeMott, Balwinder Singh, Kai Zhang, Po-Lun Ma, Mingxuan Wu, Hailong Wang, Simon P. Alexander, and Susannah M. Burrows
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Liji M. David, Mary Barth, Lena Höglund-Isaksson, Pallav Purohit, Guus J. M. Velders, Sam Glaser, and A. R. Ravishankara
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Clémence Rose, Nadine Chaumerliac, Laurent Deguillaume, Hélène Perroux, Camille Mouchel-Vallon, Maud Leriche, Luc Patryl, and Patrick Armand
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A detailed aqueous phase mechanism CLEPS 1.1 is coupled with warm microphysics including activation of aerosol particles into cloud droplets. Simulated aqueous concentrations of carboxylic acids are close to the long-term measurements conducted at Puy de Dôme (France). Sensitivity tests show that formic and acetic acids mainly originate from the gas phase with highly variable aqueous-phase reactivity depending on cloud pH, while C3–C4 carboxylic acids mainly originate from the particulate phase.
R. Mashayekhi and J. J. Sloan
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C. A. Klich and H. E. Fuelberg
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J.-F. Doussin and A. Monod
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C. Mouchel-Vallon, P. Bräuer, M. Camredon, R. Valorso, S. Madronich, H. Herrmann, and B. Aumont
Atmos. Chem. Phys., 13, 1023–1037, https://doi.org/10.5194/acp-13-1023-2013, https://doi.org/10.5194/acp-13-1023-2013, 2013
H. S. Peterson and W. H. Beasley
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W. Feng, M. P. Chipperfield, S. Dhomse, B. M. Monge-Sanz, X. Yang, K. Zhang, and M. Ramonet
Atmos. Chem. Phys., 11, 5783–5803, https://doi.org/10.5194/acp-11-5783-2011, https://doi.org/10.5194/acp-11-5783-2011, 2011
M. Bangert, C. Kottmeier, B. Vogel, and H. Vogel
Atmos. Chem. Phys., 11, 4411–4423, https://doi.org/10.5194/acp-11-4411-2011, https://doi.org/10.5194/acp-11-4411-2011, 2011
M. R. Russo, V. Marécal, C. R. Hoyle, J. Arteta, C. Chemel, M. P. Chipperfield, O. Dessens, W. Feng, J. S. Hosking, P. J. Telford, O. Wild, X. Yang, and J. A. Pyle
Atmos. Chem. Phys., 11, 2765–2786, https://doi.org/10.5194/acp-11-2765-2011, https://doi.org/10.5194/acp-11-2765-2011, 2011
T. Raventos-Duran, M. Camredon, R. Valorso, C. Mouchel-Vallon, and B. Aumont
Atmos. Chem. Phys., 10, 7643–7654, https://doi.org/10.5194/acp-10-7643-2010, https://doi.org/10.5194/acp-10-7643-2010, 2010
H. Tost, M. G. Lawrence, C. Brühl, P. Jöckel, The GABRIEL Team, and The SCOUT-O3-DARWIN/ACTIVE Team
Atmos. Chem. Phys., 10, 1931–1951, https://doi.org/10.5194/acp-10-1931-2010, https://doi.org/10.5194/acp-10-1931-2010, 2010
H. E. Fuelberg, D. L. Harrigan, and W. Sessions
Atmos. Chem. Phys., 10, 817–842, https://doi.org/10.5194/acp-10-817-2010, https://doi.org/10.5194/acp-10-817-2010, 2010
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Short summary
This paper describes the process of the transfer of water molecules between liquid and the ice during the early stages of ice formation. Using concepts of nonreversible thermodynamics, it is shown that the activation energy can be defined in terms of the bulk self-diffusivity of water and the probability of interface transfer. The application of this model to classical nucleation theory shows good agreement of measured nucleation rates with experimental results for temperatures as low as 190K.
This paper describes the process of the transfer of water molecules between liquid and the ice...
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