Heterogeneous nucleation of ice particles on glassy aerosols under cirrus conditions

Murray, Benjamin J.; Wilson, T. W.; Dobbie, S.; Cui, Zhiqiang; Al-Jumur, Sardar M. R. K.; Möhler, Ottmar; Schnaiter, M.; Wagner, Robert; Benz, Stefan; Niemand, M.; Saathoff, H.; Ebert, Volker; Wagner, Steven; Kärcher, B.

doi:10.1038/ngeo817

Cited by 320 publications

(402 citation statements)

References 27 publications

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“…The situation may, however, be different for solutes at high concentration, which impede or even prevent any water crystallization at temperatures even far below the melting point (55). Numerous references are made to "ice I c " in atmospheric science, in particular in the context of cirrus clouds (20,31,33,56,57). The possible presence of "ice I c " is generally considered in the short life cycles of such clouds and has been studied in some detail in laboratory work (8,20,33,55,58,59) and molecular-scale computer simulations of freezing of supercooled water (8,(60)(61)(62).…”

Section: Discussionmentioning

confidence: 99%

Extent and relevance of stacking disorder in “ice I_c”

Kuhs

Sippel

Falenty

et al. 2012

Proc. Natl. Acad. Sci. U.S.A.

212

280

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A solid water phase commonly known as "cubic ice" or "ice I c " is frequently encountered in various transitions between the solid, liquid, and gaseous phases of the water substance. It may form, e.g., by water freezing or vapor deposition in the Earth's atmosphere or in extraterrestrial environments, and plays a central role in various cryopreservation techniques; its formation is observed over a wide temperature range from about 120 K up to the melting point of ice. There was multiple and compelling evidence in the past that this phase is not truly cubic but composed of disordered cubic and hexagonal stacking sequences. The complexity of the stacking disorder, however, appears to have been largely overlooked in most of the literature. By analyzing neutron diffraction data with our stacking-disorder model, we show that correlations between next-nearest layers are clearly developed, leading to marked deviations from a simple random stacking in almost all investigated cases. We follow the evolution of the stacking disorder as a function of time and temperature at conditions relevant to atmospheric processes; a continuous transformation toward normal hexagonal ice is observed. We establish a quantitative link between the crystallite size established by diffraction and electron microscopic images of the material; the crystallite size evolves from several nanometers into the micrometer range with progressive annealing. The crystallites are isometric with markedly rough surfaces parallel to the stacking direction, which has implications for atmospheric sciences.

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Section: Discussionmentioning

confidence: 99%

Extent and relevance of stacking disorder in “ice I_c”

Kuhs

Sippel

Falenty

et al. 2012

Proc. Natl. Acad. Sci. U.S.A.

212

280

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“…1C) and are large enough (0.25-1 μm, SI Appendix, Table S2) to support IN activity (25). Given also that many species (especially Proteobacteria) are known to be efficient nuclei for the formation of water droplets and ice crystals, and that middle-toupper troposphere (e.g., low temperature) clouds can be affected by low-activity IN (26), airborne bacterial cells could influence cloud formation and precipitation more than previously thought. Furthermore, about 85% of the total SSU rRNA gene sequences that were recovered from the GRIP samples and were assignable to a habitat on Earth represented aquatic species (Fig.…”

Section: Discussionmentioning

confidence: 99%

Microbiome of the upper troposphere: Species composition and prevalence, effects of tropical storms, and atmospheric implications

DeLeon-Rodriguez¹,

Lathem²,

Rodriguez-R³

et al. 2013

Proc. Natl. Acad. Sci. U.S.A.

381

308

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The composition and prevalence of microorganisms in the middle-toupper troposphere (8-15 km altitude) and their role in aerosol-cloudprecipitation interactions represent important, unresolved questions for biological and atmospheric science. In particular, airborne microorganisms above the oceans remain essentially uncharacterized, as most work to date is restricted to samples taken near the Earth's surface. Here we report on the microbiome of low-and high-altitude air masses sampled onboard the National Aeronautics and Space Administration DC-8 platform during the 2010 Genesis and Rapid Intensification Processes campaign in the Caribbean Sea. The samples were collected in cloudy and cloud-free air masses before, during, and after two major tropical hurricanes, Earl and Karl. Quantitative PCR and microscopy revealed that viable bacterial cells represented on average around 20% of the total particles in the 0.25-to 1-μm diameter range and were at least an order of magnitude more abundant than fungal cells, suggesting that bacteria represent an important and underestimated fraction of micrometer-sized atmospheric aerosols. The samples from the two hurricanes were characterized by significantly different bacterial communities, revealing that hurricanes aerosolize a large amount of new cells. Nonetheless, 17 bacterial taxa, including taxa that are known to use C1-C4 carbon compounds present in the atmosphere, were found in all samples, indicating that these organisms possess traits that allow survival in the troposphere. The findings presented here suggest that the microbiome is a dynamic and underappreciated aspect of the upper troposphere with potentially important impacts on the hydrological cycle, clouds, and climate.ice nucleation | cloud condensation nuclei | microbial community | pyrosequencing | biogeography

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“…40,43 As a consequence, glassy organicinorganic aerosol particles (not fully equilibrated with the ambient RH) may act preferentially as heterogeneous ice nuclei, rather than as cloud condensation nuclei forming liquid water droplets. 44,45 …”

Section: Hygroscopic Growth Timescale Of Soamentioning

confidence: 99%

Gas–particle partitioning of atmospheric aerosols: interplay of physical state, non-ideal mixing and morphology

Shiraiwa

Zuend

Bertram

et al. 2013

Phys. Chem. Chem. Phys.

246

268

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Atmospheric aerosols, comprising organic compounds and inorganic salts, play a key role in air quality and climate. Mounting evidence exists that these particles frequently exhibit phase separation into predominantly organic and aqueous electrolyte-rich phases. As well, the presence of amorphous semi-solid or glassy particle phases has been established. Using the canonical system of ammonium sulfate mixed with organics from the ozone oxidation of a-pinene, we illustrate theoretically the interplay of physical state, non-ideality, and particle morphology affecting aerosol mass concentration and the characteristic timescale of gas-particle mass transfer. Phase separation can significantly affect overall particle mass and chemical composition. Semi-solid or glassy phases can kinetically inhibit the partitioning of semivolatile components and hygroscopic growth, in contrast to the traditional assumption that organic compounds exist in quasi-instantaneous gas-particle equilibrium. These effects have significant implications for the interpretation of laboratory data and the development of improved atmospheric air quality and climate models.

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Heterogeneous nucleation of ice particles on glassy aerosols under cirrus conditions

Cited by 320 publications

References 27 publications

Extent and relevance of stacking disorder in “ice I_c”

Extent and relevance of stacking disorder in “ice I_c”

Microbiome of the upper troposphere: Species composition and prevalence, effects of tropical storms, and atmospheric implications

Gas–particle partitioning of atmospheric aerosols: interplay of physical state, non-ideal mixing and morphology

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Heterogeneous nucleation of ice particles on glassy aerosols under cirrus conditions

Cited by 320 publications

References 27 publications

Extent and relevance of stacking disorder in “ice Ic”

Extent and relevance of stacking disorder in “ice Ic”

Microbiome of the upper troposphere: Species composition and prevalence, effects of tropical storms, and atmospheric implications

Gas–particle partitioning of atmospheric aerosols: interplay of physical state, non-ideal mixing and morphology

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Extent and relevance of stacking disorder in “ice I_c”

Extent and relevance of stacking disorder in “ice I_c”