Ambient concentrations of ice-forming particles measured during ship expeditions are collected and summarised with the aim of determining the spatial distribution and variability in ice nuclei in ...oceanic regions.
The presented data from literature and previously unpublished data from over 23 months of ship-based measurements stretch from the Arctic to the Southern Ocean and include a circumnavigation of Antarctica. In comparison to continental observations, ship-based measurements of ambient ice nuclei show 1 to 2 orders of magnitude lower mean concentrations. To quantify the geographical variability in oceanic areas, the concentration range of potential ice nuclei in different climate zones is analysed by meridionally dividing the expedition tracks into tropical, temperate and polar climate zones. We find that concentrations of ice nuclei in these meridional zones follow temperature spectra with similar slopes but vary in absolute concentration. Typically, the frequency with which specific concentrations of ice nuclei are observed at a certain temperature follows a log-normal distribution. A consequence of the log-normal distribution is that the mean concentration is higher than the most frequently measured concentration. Finally, the potential contribution of ship exhaust to the measured ice nuclei concentration on board research vessels is analysed as function of temperature. We find a sharp onset of the influence at approximately −36 ∘C but none at warmer temperatures that could bias ship-based measurements.
Black carbon (BC) aerosol plays an important role in the Earth’s climate system because it absorbs solar radiation and therefore potentially warms the climate; however, BC can also act as a seed for ...cloud particles, which may offset much of its warming potential. If BC acts as an ice nucleating particle (INP), BC could affect the lifetime, albedo, and radiative properties of clouds containing both supercooled liquid water droplets and ice particles (mixed-phase clouds). Over 40% of global BC emissions are from biomass burning; however, the ability of biomass burning BC to act as an INP in mixed-phase cloud conditions is almost entirely unconstrained. To provide these observational constraints, we measured the contribution of BC to INP concentrations (INP) in real-world prescribed burns and wildfires. We found that BC contributes, at most, 10% to INP during these burns. From this, we developed a parameterization for biomass burning BC and combined it with a BC parameterization previously used for fossil fuel emissions. Applying these parameterizations to global model output, we find that the contribution of BC to potential INP relevant to mixed-phase clouds is ∼5% on a global average.
A number of new measurement methods for ice nucleating particles (INPs) have been introduced in recent years, and it is important to address how these methods compare. Laboratory comparisons of ...instruments sampling major INP types are common, but few comparisons have occurred for ambient aerosol measurements exploring the utility, consistency and complementarity of different methods to cover the large dynamic range of INP concentrations that exists in the atmosphere. In this study, we assess the comparability of four offline immersion freezing measurement methods (Colorado State University ice spectrometer, IS; North Carolina State University cold stage, CS; National Institute for Polar Research Cryogenic Refrigerator Applied to Freezing Test, CRAFT; University of British Columbia micro-orifice uniform deposit impactor–droplet freezing technique, MOUDI-DFT) and an online method (continuous flow diffusion chamber, CFDC) used in a manner deemed to promote/maximize immersion freezing, for the detection of INPs in ambient aerosols at different locations and in different sampling scenarios. We also investigated the comparability of different aerosol collection methods used with offline immersion freezing instruments. Excellent agreement between all methods could be obtained for several cases of co-sampling with perfect temporal overlap. Even for sampling periods that were not fully equivalent, the deviations between atmospheric INP number concentrations measured with different methods were mostly less than 1 order of magnitude. In some cases, however, the deviations were larger and not explicable without sampling and measurement artifacts. Overall, the immersion freezing methods seem to effectively capture INPs that activate as single particles in the modestly supercooled temperature regime (> −20 °C), although more comparisons are needed in this temperature regime that is difficult to access with online methods. Relative to the CFDC method, three immersion freezing methods that disperse particles into a bulk liquid (IS, CS, CRAFT) exhibit a positive bias in measured INP number concentrations below −20 °C, increasing with decreasing temperature. This bias was present but much less pronounced for a method that condenses separate water droplets onto limited numbers of particles prior to cooling and freezing (MOUDI-DFT). Potential reasons for the observed differences are discussed, and further investigations proposed to elucidate the role of all factors involved.
Black carbon (BC) aerosol plays an important role in the Earth’s climate system because it absorbs solar radiation and therefore potentially warms the climate; however, BC can also act as a seed for ...cloud particles, which may offset much of its warming potential. If BC acts as an ice nucleating particle (INP), BC could affect the lifetime, albedo, and radiative properties of clouds containing both supercooled liquid water droplets and ice particles (mixed-phase clouds). Over 40% of global BC emissions are from biomass burning; however, the ability of biomass burning BC to act as an INP in mixed-phase cloud conditions is almost entirely unconstrained. To provide these observational constraints, we measured the contribution of BC to INP concentrations (INP) in real-world prescribed burns and wildfires. We found that BC contributes, at most, 10% to INP during these burns. From this, we developed a parameterization for biomass burning BC and combined it with a BC parameterization previously used for fossil fuel emissions. Applying these parameterizations to global model output, we find that the contribution of BC to potential INP relevant to mixed-phase clouds is ~5% on a global average.
The role of marine ice-nucleating particles (INPs) in modifying clouds and radiation balance over oceans is uncertain. While recent studies have advanced our understanding of the abundance of marine ...INPs, characterizing their sources and composition remains a challenge. INP concentrations above oceans are typically low, sometimes extraordinarily so, but there is evidence of elevated levels associated with phytoplankton blooms. Mesocosm experiments have shown that ice-nucleating entities (INEs, which include discrete particles as well as ice-nucleating monolayers) are produced, and INP emissions raised, in the decay phase following bloom collapse. To test if INE production depends upon phytoplankton type, we added dead particulate biomass of a green alga (
Nannochloris atomus
), a diatom (
Skeletonema marinoi
) and a cyanobacterium (
Prochlorococcus marinus
) to a miniature Marine Aerosol Reference Tank filled with seawater. As decomposition progressed, heterotrophic bacteria initially increased and plateaued, then declined, coinciding with an increase in heterotrophic nanoflagellates (HNF) and viruses. Enzyme activities typically increased over several days before plateauing or decreasing, while humic-like substances (HULIS) steadily accumulated. INEs in the seawater peaked 3-5 days after each detritus addition, increasing ∼10- to ∼20-fold. INE concentration was closely correlated with HNF counts, viruses and the concentration of HULIS, but not with bacteria or enzyme activities. Newly-fabricated INEs were organic, primarily heat stable (95 °C), and varied in size. INP concentrations in sea spray aerosol (SSA) tended to peak shortly before the peak of INEs in the seawater, at 4-, 35- and 15-fold higher than at the start in the
N. atomus
,
S. marinoi
, and
P. marinus
incubations, respectively. Using data from the
P. marinus
incubation, we were able to provide the first estimate of INP enrichment in SSA (over its concentration in the water): it was initially ∼200× for the fresh seawater and increased further after the addition of the
P. marinus
inoculum. We also tested if a simple nutrient mix (bovine serum albumin (BSA) and three monosaccharides) could stimulate INP production: INEs in the seawater changed little, but INP emissions fell abruptly immediately upon BSA addition due to it forming a monolayer which displaced the sea surface microlayer (SML). These experiments revealed that INE production in the decay phase of a phytoplankton bloom requires the addition of a natural, complex substrate to initiate a realistic succession of decomposers, and that INP emissions are further controlled by their concentration in the SML and, indirectly, by the impact of SML composition upon jet and film drop production.
Oceans emit ice-nucleating particles (INPs) which freeze supercooled cloud droplets, modifying clouds. We added dead biomass of three phytoplankton to seawater. Each time, this stimulated INP production in the water and INP emissions in sea spray.
PDF
