When Do Subpollen Particles Become Relevant for Ice Nucleation Processes in Clouds?

When exposed to sufficiently humid environments, pollen grains burst and release large quantities of small subpollen particles (SPPs) which carry ice nucleating macromolecules. In this study, for the first time we develop a physically based parameterization describing the bursting process of pollen by applying a turgor pressure parameterization and quantify the impact SPPs have on overall ice nucleation in clouds. SPPs are generated from simulated birch pollen emissions over Europe for a 10-day case study in spring. We found SPP concentrations to surpass pollen grain concentrations by 4–6 orders of magnitude leading to an abundance of biological ice nuclei from SPPs in the range of 103−104\ua0m−3. However, it is found that these concentrations lead to only small changes in hydrometeor number densities and precipitation. Addressing the question when SPPs become relevant for ice nucleation in clouds, we conducted a sensitivity investigation. We find that amplifying ice nucleation efficiency of biological particles by factors greater 100 increases the ice particle numbers by up to 25% (T\ua0≈\ua0268\ua0K). Strong reductions show in cloud droplet number concentration and water vapor at these temperatures while water vapor is increasing at 600\ua0m. Overall, we found a net reduction of water in the atmosphere as liquid and particularly water vapor density is reduced, while frozen water mass density increases above 257\ua0K. Findings indicate an alteration of mixed-phase cloud composition and increased precipitation (up to 6.2%) when SPPs are considered as highly efficient biological ice nuclei

Condensation/immersion mode ice-nucleating particles in a boreal environment

Ice-nucleating particle (INP) measurements were performed in the boreal environment of southern Finland at the Station for Measuring Ecosystem-Atmosphere Relations (SMEAR II) in the winter-spring of 2018. Measurements with the Portable Ice Nucleation Chamber (PINC) were conducted at 242 K and 105 % relative humidity with respect to water. The median INP number concentration [INP] during a 6-week measurement period was 13 L-1. The [INP] spanned 3 orders of magnitude and showed a general increase from mid-February until early April. No single dominant local or regional sources of INPs in the boreal environment of southern Finland could be identified. Rather, it is hypothesised that the INPs detected at SMEAR II are a result of long-range transport and dilution of INPs sourced far from the measurement site. Despite high variability, the measured [INP] values fall within the range expected for the [INP] measured elsewhere under similar thermodynamic conditions. The [INP] did not correlate with any of the examined parameters during the entire field campaign, indicating that no one single parameter can be used to predict the [INP] at the measurement location during the examined time period. The absence of a correlation across the entire field campaign also suggests that a variety of particles act as INPs at different times, although it was indirectly determined that ambient INPs are most likely within the size range of 0.1-0.5 mu m in diameter on average. On shorter timescales, several particle species correlated well with the [INP]. Depending on the meteorological conditions, black carbon (BC), supermicron biological particles and sub-0.1 mu m particles, most likely nanoscale biological fragments such as ice-nucleating macromolecules (INMs), correlated with the INP signal. However, an increase in the concentration of any of these particle species may not necessarily lead to the increase in the [INP]; the reasons for this remain unknown. Limitations of the instrumental set-up and the necessity for future field INP studies are addressed.Peer reviewe

Background Free‐Tropospheric Ice Nucleating Particle Concentrations at Mixed‐Phase Cloud Conditions

Clouds containing ice are vital for precipitation formation and are important in determining the Earths radiative budget. However primary formation of ice in clouds is not fully understood. In the presence of ice nucleating particles (INPs), the phase change to ice is promoted, but identification and quantification of INPs in a natural environment remains challenging because of their low numbers. In this paper we quantify INP number concentrations in the free troposphere (FT) as measured at the High Altitude Research Station Jungfraujoch during the years 2014 to 2017. INPs were measured at conditions relevant for mixed-phase cloud formation at 241 to 242 K

Measurement report : Introduction to the HyICE-2018 campaign for measurements of ice-nucleating particles and instrument inter-comparison in the Hyytiala boreal forest

The formation of ice particles in Earth's atmosphere strongly influences the dynamics and optical properties of clouds and their impacts on the climate system. Ice formation in clouds is often triggered heterogeneously by ice-nucleating particles (INPs) that represent a very low number of particles in the atmosphere. To date, many sources of INPs, such as mineral and soil dust, have been investigated and identified in the low and mid latitudes. Although less is known about the sources of ice nucleation at high latitudes, efforts have been made to identify the sources of INPs in the Arctic and boreal environments. In this study, we investigate the INP emission potential from high-latitude boreal forests in the mixed-phase cloud regime. We introduce the HyICE-2018 measurement campaign conducted in the boreal forest of Hyytiala, Finland, between February and June 2018. The campaign utilized the infrastructure of the Station for Measuring Ecosystem-Atmosphere Relations (SMEAR) II, with additional INP instruments, including the Portable Ice Nucleation Chamber I and II (PINC and PINCii), the SPectrometer for Ice Nuclei (SPIN), the Portable Ice Nucleation Experiment (PINE), the Ice Nucleation SpEctrometer of the Karlsruhe Institute of Technology (INSEKT) and the Microlitre Nucleation by Immersed Particle Instrument (mu L-NIPI), used to quantify the INP concentrations and sources in the boreal environment. In this contribution, we describe the measurement infrastructure and operating procedures during HyICE-2018, and we report results from specific time periods where INP instruments were run in parallel for inter-comparison purposes. Our results show that the suite of instruments deployed during HyICE-2018 reports consistent results and therefore lays the foundation for forthcoming results to be considered holistically. In addition, we compare measured INP concentrations to INP parameterizations, and we observe good agreement with the Tobo et al. (2013) parameterization developed from measurements conducted in a ponderosa pine forest ecosystem in Colorado, USA.Peer reviewe

Measurement report : Introduction to the HyICE-2018 campaign for measurements of ice-nucleating particles and instrument inter-comparison in the Hyytiala boreal forest

The formation of ice particles in Earth's atmosphere strongly influences the dynamics and optical properties of clouds and their impacts on the climate system. Ice formation in clouds is often triggered heterogeneously by ice-nucleating particles (INPs) that represent a very low number of particles in the atmosphere. To date, many sources of INPs, such as mineral and soil dust, have been investigated and identified in the low and mid latitudes. Although less is known about the sources of ice nucleation at high latitudes, efforts have been made to identify the sources of INPs in the Arctic and boreal environments. In this study, we investigate the INP emission potential from high-latitude boreal forests in the mixed-phase cloud regime. We introduce the HyICE-2018 measurement campaign conducted in the boreal forest of Hyytiala, Finland, between February and June 2018. The campaign utilized the infrastructure of the Station for Measuring Ecosystem-Atmosphere Relations (SMEAR) II, with additional INP instruments, including the Portable Ice Nucleation Chamber I and II (PINC and PINCii), the SPectrometer for Ice Nuclei (SPIN), the Portable Ice Nucleation Experiment (PINE), the Ice Nucleation SpEctrometer of the Karlsruhe Institute of Technology (INSEKT) and the Microlitre Nucleation by Immersed Particle Instrument (mu L-NIPI), used to quantify the INP concentrations and sources in the boreal environment. In this contribution, we describe the measurement infrastructure and operating procedures during HyICE-2018, and we report results from specific time periods where INP instruments were run in parallel for inter-comparison purposes. Our results show that the suite of instruments deployed during HyICE-2018 reports consistent results and therefore lays the foundation for forthcoming results to be considered holistically. In addition, we compare measured INP concentrations to INP parameterizations, and we observe good agreement with the Tobo et al. (2013) parameterization developed from measurements conducted in a ponderosa pine forest ecosystem in Colorado, USA.Peer reviewe

Pollen Ice Nucleating Particles and Their Response to Atmospheric Processing

Clouds are crucial to life on Earth as they help regulate temperature and distribute water resources. Yet, large uncertainties exist around cloud development and evolution with many open questions about processes spanning from micro- to macro-scales. On the micro-scale, ice formation contributes to precipitation formation and cloud radiative properties; yet our understanding of this process is limited. This thesis assesses the ice nucleating (IN) ability of pollen and subpollen particles (SPPs) under mixed-phase and cold cloud conditions. In a first step, pollen IN activity was investigated under mixed-phase cloud conditions where IN activity was found to vary between pollen types and that submicron SPPs drive pollen IN activity. Additionally, one pollen type, grey alder, was identified to initiate freezing above −10°C, thus contributing to a small set of highly active ice nucleating particles (INPs). In a second step, atmospheric processing of SPPs was investigated, as SPPs can experience atmospheric transport and exposure to varying environmental conditions. Several processing pathways were found to compromise pollen IN activity. The largest impacts were observed for the most IN active pollen by exposure to simulated solar radiation. Under cold cloud conditions, chemical oxidation negatively impacts the IN activity of silver birch and grey alder pollen, occurring on a similar timescale as changes to the molecular structure were observed. The findings from laboratory INP measurements were translated to parametrize INP concentrations from SPPs, indicating INP concentrations below 10-2 m-3 in one modeling scenario. To overcome potential barriers in detecting such low INP concentrations by commonly used INP instruments, a Portable Fine Particle Concentrator was evaluated for INP measurements in the field. Enrichment factors are found to be particle size dependent while an INP enrichment factor of 16±5 was achieved in a mountain-top field study. The insights gained from this thesis will help assess the importance of pollen as INPs and reduce uncertainties that cloud processes currently impose on weather and climate predictions.Ph.D

Oxidative Processing Lowers the Ice Nucleation Activity of Birch and Alder Pollen

Pollen carry water extractable compounds with ice nucleating (IN) activity. This study investigates whether the hydroxyl radical, as the major atmospheric oxidant, can affect the IN activity of silver birch and grey alder subpollen particles under in-cloud conditions for deposition freezing mode conditions at 234 K. It is found that oxidation increases the supersaturation ratio with respect to ice necessary for the onset of ice nucleation and decreases the fraction of particles which initiate ice nucleation. This reduction of IN activity under equivalent oxidation conditions does not occur with a mineral dust sample (Arizona Test Dust). Chemical analysis of fresh and oxidized pollen material indicates a change of molecular structure with a loss of conjugation and an increase in oxidized functional groups, such as carbonyls. This is the first demonstration that in-cloud oxidation may lower the IN abilities of biological particles such as pollen.The authors would like to acknowledge the Natural Sciences and Engineering Research Council (NSERC) for funding under grant RGPIN-2017-05972. The authors declare no conflict of interest regarding affiliation or funding. We acknowledge Z. Dráb from Pharmallerga for providing the pollen. Figure source data for all plots shown in this publication have been deposited in the University of Toronto Dataverse (doi:10.5683/SP/JLPHBI; Gute & Abbatt, 2018

Background Free-Tropospheric Ice Nucleating Particle Concentrations at Mixed-Phase Cloud Conditions

Clouds containing ice are vital for precipitation formation and are important in determining the Earths radiative budget. However primary formation of ice in clouds is not fully understood. In the presence of ice nucleating particles (INPs), the phase change to ice is promoted, but identification and quantification of INPs in a natural environment remains challenging because of their low numbers. In this paper we quantify INP number concentrations in the free troposphere (FT) as measured at the High Altitude Research Station Jungfraujoch during the years 2014 to 2017. INPs were measured at conditions relevant for mixed-phase cloud formation at 241 to 242 K

Background Free-Tropospheric Ice Nucleating Particle Concentrations at Mixed-Phase Cloud Conditions

Clouds containing ice are vital for precipitation formation and are important in determining the Earth's radiative budget. However, primary formation of ice in clouds is not fully understood. In the presence of ice nucleating particles (INPs), the phase change to ice is promoted, but identification and quantification of INPs in a natural environment remains challenging because of their low numbers. In this paper, we quantify INP number concentrations in the free troposphere (FT) as measured at the High Altitude Research Station Jungfraujoch (JFJ), during the winter, spring, and summer of the years 2014–2017. INPs were measured at conditions relevant for mixed‐phase cloud formation at T = 241/242 K. To date, this is the longest timeline of semiregular measurements akin to online INP monitoring at this site and sampling conditions. We find that INP concentrations in the background FT are on average capped at 10/stdL (liter of air at standard conditions [T = 273 K and p = 1013 hPa]) with an interquartile range of 0.4–9.6/stdL, as compared to measurements during times when other air mass origins (e.g., Sahara or marine boundary layer) prevailed. Elevated concentrations were measured in the field campaigns of 2016, which might be due to enhanced influence from Saharan dust and marine boundary layer air arriving at the JFJ. The upper limit of INP concentrations in the background FT is supported by measurements performed at similar conditions, but at different locations in the FT, where we find INP concentrations to be below 13/stdL most of the time.ISSN:0148-0227ISSN:2169-897