Search

Cloud properties are strongly influenced by ice formation; hence, we need to understand the sources of ice-nucleating particles (INPs) around the globe. Boreal forests are known as sources of bioaerosol, and recent work indicates that these dominate the INP spectra above - 24 °C. To quantify the INP population at temperatures below - 24 °C , we deployed a portable cloud expansion chamber (PINE) in a Finnish boreal forest from 13 March 2018 to 11 May 2018. Using the 6 min time resolution PINE data, we present several lines of evidence that INPs below - 24 °C in this location are also from biological sources: (i) an INP parameterization developed for a pine forest site in Colorado, where many INPs were shown to be biological, produced a good fit to our measurements; a moderate correlation of INPs with aerosol concentration larger than 0.5 µm and the fluorescent bioaerosol concentration; (ii) a negative correlation with relative humidity that may relate to enhanced release of bioaerosol at low humidity from local sources such as the prolific lichen population in boreal forests; and (iii) the absence of correlation with ultra-fine particles (3.5 to 50 nm), indicating that new particle formation events are not sources of INPs. This study should motivate further work to establish whether the commonality in bioaerosol ice-nucleating properties between spring in Finland and summer in Colorado is more generally applicable to different coniferous forest locations and times and also to determine to what extent these bioaerosols are transported to locations where they may affect clouds. [ABSTRACT FROM AUTHOR]

Ice nucleating particles (INPs) play a crucial role in initiating ice crystal formation in clouds, influencing the dynamics and optical properties of clouds and their impacts on precipitation and the climate system. Despite their importance, there is limited knowledge about the vertical distribution of INPs. This study focuses on aircraft measurements conducted during spring 2018 above the boreal forest of Hyytiälä, Finland. Similarities between INP concentrations, activated fractions, particle concentrations, and size distributions observed at ground level and in the boundary layer aloft indicate that surface particles and INPs are efficiently transported and mixed within the boundary layer. INP concentrations observed in the boundary layer are best predicted by a parameterization describing near-surface INP concentrations driven by the abundance of biogenic aerosol in the Finnish boreal forest, suggesting that biogenic INPs are dominant in the boundary layer above the same environment. Most of the INP concentrations and activated fractions observed in the free troposphere are notably lower than in the boundary layer, and the distinct particle size distributions suggest that different aerosol populations, likely resulting from long-range transport, are present in the free troposphere. However, we show one case where higher INP concentrations are observed in the free troposphere and where a homogeneous particle population exists from the surface to the free troposphere. This indicates that surface particles and INPs from the boreal forest can occasionally reach the free troposphere, which is particularly important as the INPs in the free troposphere can further travel horizontally and/or vertically and impact cloud formation. [ABSTRACT FROM AUTHOR]

Ice-nucleating particle concentrations (INPCs) can spread over several orders of magnitude at any given temperature. However, this variability is rarely accounted for in heterogeneous ice-nucleation parameterizations. In this paper, we present an approach to incorporate the random variation in the INPC into the parameterization of immersion freezing and analyze this novel concept with various sensitivity tests. In the new scheme, the INPC is drawn from a relative frequency distribution of cumulative INPCs. At each temperature, this distribution describing the INPCs is expressed as a lognormal frequency distribution. The new parameterization scheme does not require aerosol information from the driving model to represent the heterogeneity of INPCs. The scheme's performance is tested in a large-eddy simulation of a relatively warm Arctic mixed-phase stratocumulus. We find that it leads to reasonable ice masses in the cloud, especially when compared to immersion freezing schemes that yield one fixed INPC per temperature and lead to almost no ice production in the simulated cloud. The scheme is sensitive to the median of the frequency distribution and highly sensitive to the standard deviation of the distribution, as well as to the frequency of drawing a new INPC and the resolution of the model. Generally, a higher probability of drawing large INPCs leads to substantially more ice in the simulated cloud. We expose inherent challenges to introducing such a parameterization and explore possible solutions and potential developments. [ABSTRACT FROM AUTHOR]

The Portable Ice Nucleation Chamber 2 (PINCii) is a newly developed continuous flow diffusion chamber (CFDC) for measuring ice nucleating particles (INPs). PINCii is a vertically oriented parallel-plate CFDC that has been engineered to improve upon the limitations of previous generations of CFDCs. This work presents a detailed description of the PINCii instrument and the upgrades that make it unique compared with other operational CFDCs. The PINCii design offers several possibilities for improved INP measurements. Notably, a specific icing procedure results in low background particle counts, which demonstrates the potential for PINCii to measure INPs at low concentrations (<10 L -1). High-spatial-resolution wall-temperature mapping enables the identification of temperature inhomogeneities on the chamber walls. This feature is used to introduce and discuss a new method for analyzing CFDC data based on the most extreme lamina conditions present within the chamber, which represent conditions most likely to trigger ice nucleation. A temperature gradient can be maintained throughout the evaporation section in addition to the main chamber, which enables PINCii to be used to study droplet activation processes or to extend ice crystal growth. A series of both liquid droplet activation and ice nucleation experiments were conducted at temperature and saturation conditions that span the spectrum of PINCii's operational conditions (-50≤ temperature ≤-15 ∘ C and 100 ≤ relative humidity with respect to ice ≤160 %) to demonstrate the instrument's capabilities. In addition, typical sources of uncertainty in CFDCs, including particle background, particle loss, and variations in aerosol lamina temperature and relative humidity, are quantified and discussed for PINCii. [ABSTRACT FROM AUTHOR]

Ice nucleating particle (INP) concentrations can spread over several orders of magnitude at any given temperature. However, this variability is rarely accounted for in heterogeneous ice nucleation parameterizations. We developed a scheme for immersion freezing where the INP concentration is drawn from a relative frequency distribution of cumulative INP concentrations. At each temperature, this distribution describing the INP concentrations is expressed as a log-normal frequency distribution. The new parameterization scheme does not require aerosol information from the driving model to represent the heterogeneity of INP concentrations. The scheme's performance is tested in a large-eddy simulation of an Arctic stratocumulus. We find that it leads to reasonable ice masses in the cloud. The scheme is sensitive to the median of the frequency distribution and highly sensitive to the standard deviation of the distribution. Generally, larger probability to draw high INP concentrations leads to substantially more ice in the simulated cloud. [ABSTRACT FROM AUTHOR]

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 Hyytiälä, 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 (µ 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 parameterization developed from measurements conducted in a ponderosa pine forest ecosystem in Colorado, USA. [ABSTRACT FROM AUTHOR]

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 lower latitudes. Although less is known about the sources of ice nucleation at higher 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. We introduce the HyICE-2018 measurement campaign conducted in the boreal forest of Hyytiälä, Finland between February and June 2018. The campaign utilized the infrastructure of the SMEAR II research station with additional instrumentation for measuring INPs to quantify the concentrations and sources of INPs 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 the INP concentration we measured to INP parameterizations, and we show a very good agreement with the Tobo et al. (2013) parameterization developed from measurements conducted in a ponderosa pine forest ecosystem in Colorado, USA. [ABSTRACT FROM AUTHOR]

Ice-nucleating particles (INPs) trigger the formation of cloud ice crystals in the atmosphere. Therefore, they strongly influence cloud microphysical and optical properties and precipitation and the life cycle of clouds. Improving weather forecasting and climate projection requires an appropriate formulation of atmospheric INP concentrations. This remains challenging as the global INP distribution and variability depend on a variety of aerosol types and sources, and neither their short-term variability nor their long-term seasonal cycles are well covered by continuous measurements. Here, we provide the first year-long set of observations with a pronounced INP seasonal cycle in a boreal forest environment. Besides the observed seasonal cycle in INP concentrations with a minimum in wintertime and maxima in early and late summer, we also provide indications for a seasonal variation in the prevalent INP type. We show that the seasonal dependency of INP concentrations and prevalent INP types is most likely driven by the abundance of biogenic aerosol. As current parameterizations do not reproduce this variability, we suggest a new mechanistic description for boreal forest environments which considers the seasonal variation in INP concentrations. For this, we use the ambient air temperature measured close to the ground at 4.2 m height as a proxy for the season, which appears to affect the source strength of biogenic emissions and, thus, the INP abundance over the boreal forest. Furthermore, we provide new INP parameterizations based on the Ice Nucleation Active Surface Site (INAS) approach, which specifically describes the ice nucleation activity of boreal aerosols particles prevalent in different seasons. Our results characterize the boreal forest as an important but variable INP source and provide new perspectives to describe these new findings in atmospheric models. [ABSTRACT FROM AUTHOR]

Ice particle activation and evolution have important atmospheric implications for cloud formation, initiation of precipitation and radiative interactions. The initial formation of atmospheric ice by heterogeneous ice nucleation requires the presence of a nucleating seed, an ice-nucleating particle (INP), to facilitate its first emergence. Unfortunately, only a few long-term measurements of INPs exist, and as a result, knowledge about geographic and seasonal variations of INP concentrations is sparse. Here we present data from nearly 2 years of INP measurements from four stations in different regions of the world: the Amazon (Brazil), the Caribbean (Martinique), central Europe (Germany) and the Arctic (Svalbard). The sites feature diverse geographical climates and ecosystems that are associated with dissimilar transport patterns, aerosol characteristics and levels of anthropogenic impact (ranging from near pristine to mostly rural). Interestingly, observed INP concentrations, which represent measurements in the deposition and condensation freezing modes, do not differ greatly from site to site but usually fall well within the same order of magnitude. Moreover, short-term variability overwhelms all long-term trends and/or seasonality in the INP concentration at all locations. An analysis of the frequency distributions of INP concentrations suggests that INPs tend to be well mixed and reflective of large-scale air mass movements. No universal physical or chemical parameter could be identified to be a causal link driving INP climatology, highlighting the complex nature of the ice nucleation process. Amazonian INP concentrations were mostly unaffected by the biomass burning season, even though aerosol concentrations increase by a factor of 10 from the wet to dry season. Caribbean INPs were positively correlated to parameters related to transported mineral dust, which is known to increase during the Northern Hemisphere summer. A wind sector analysis revealed the absence of an anthropogenic impact on average INP concentrations at the site in central Europe. Likewise, no Arctic haze influence was observed on INPs at the Arctic site, where low concentrations were generally measured. We consider the collected data to be a unique resource for the community that illustrates some of the challenges and knowledge gaps of the field in general, while specifically highlighting the need for more long-term observations of INPs worldwide. [ABSTRACT FROM AUTHOR]

Ice particle activation and evolution have important atmospheric implications for cloud formation, initiation of precipitation and radiative interactions. In many cases the initial formation of atmospheric ice requires the presence of a nucleating seed, an ice nucleating particle (INP), to facilitate its first emergence. Unfortunately, few long-term measurements of INPs exist and as a result, knowledge about geographic and seasonal variations of INP concentrations is sparse. Here we present data from nearly two years of INP measurements from four stations in different regions of the world: the Amazon, the Caribbean, Central Europe and the Norwegian Arctic. The sites feature diverse geographical climates and ecosystems that are associated with dissimilar transport patterns, aerosol characteristics and levels of anthropogenic impact (ranging from near pristine to mostly rural). Interestingly, observed INP concentrations do not differ greatly from site to site, but usually fall well within the same order of magnitude. Moreover, short-term variability overwhelms all long-term trends and/or seasonality in the INP concentration at all locations. An analysis of the frequency distributions of INP concentrations suggests that INPs tend to be well-mixed and reflective of large-scale air mass movements. No universal physical or chemical parameter could be identified to be a causal link driving INP climatology, highlighting the complex nature of the ice nucleation process. Amazonian INP concentrations were mostly unaffected by the biomass burning season, even though aerosol concentrations increase by a factor of 10 from the wet to dry season. Caribbean INPs were positively correlated to parameters related to transported mineral dust, which is known to increase during the northern hemispheric summer. A wind sector analysis revealed the absence of an anthropogenic impact on average INP concentrations at the Central European site. Likewise, no Arctic Haze influence was observed on INPs at the Norwegian site, where low concentrations were generally measured. We consider the collected data to be a unique resource for the community that illustrates some of the challenges and knowledge gaps of the field in general, while specifically highlighting the need for more long-term observations of INPs worldwide. [ABSTRACT FROM AUTHOR]

Ice-nucleating particles (INPs) trigger the formation of cloud ice crystals in the atmosphere. Therefore, they strongly influence cloud microphysical and optical properties, as well as precipitation and the life cycle of clouds. Improving weather forecasting and climate projection requires an appropriate formulation of atmospheric INP concentrations. This remains challenging, as the global INP distribution and variability depend on a variety of aerosol types and sources, and neither their short-term variability nor their long-term seasonal cycles are well covered by continuous measurements. Here, we provide the first year-long set of observations with a pronounced INP seasonal cycle in a boreal forest environment. Besides the observed seasonal cycle in INP concentrations with a minimum in wintertime and maxima in early and late summer, we also provide indications for a seasonal variation in the prevalent INP type. We show that the seasonal dependency of INP concentrations and prevalent INP types is most likely driven by the abundance of biogenic aerosol. As current parameterizations do not reproduce this variability, we suggest a new parameterization approach, which considers the seasonal variation of INP concentrations. For this, we use the ambient air temperature as a proxy for the season which affects the source strength of biogenic emissions and by that the INP abundance over the boreal forest areas. Furthermore, we provide new INP parameterizations based on the Ice Nucleation Active Surface Site (INAS) approach, which specifically describes the ice nucleation activity of boreal aerosols particles prevalent in different seasons. Our results characterize the boreal forest as an important but variable INP source and provide new perspectives to describe these new findings in atmospheric models. [ABSTRACT FROM AUTHOR]

The phase state of atmospheric particulate is important to atmospheric processes, and aerosol radiative forcing remains a large uncertainty in climate predictions. That said, precise atmospheric phase behavior is difficult to quantify and observations have shown that "precondensation" of water below predicted saturation values can occur. We propose a revised approach to understanding the transition from solid soluble particles to liquid droplets, typically described as cloud condensation nucleation -- a process that is traditionally captured by Köhler theory, which describes a modified equilibrium saturation vapor pressure due to (i) mixing entropy (Raoult's law) and (ii) droplet geometry (Kelvin effect). Given that observations of precondensation are not predicted by Köhler theory, we devise a more complete model that includes interfacial forces giving rise to predeliquescence, i.e., the formation of a brine layer wetting a salt particle at relative humidities well below the deliquescence point. [ABSTRACT FROM AUTHOR]

The Nordic Centre of Excellence CRAICC (CRyosphere-Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011-2016, was the largest joint Nordic research and innovation initiative to date, aiming to strengthen research and innovation regarding climate change issues in the Nordic Region. CRAICC gathered more than 100 scientists from all Nordic countries in a virtual Centre with the objectives to identify and quantify the major processes controlling Arctic warming and related feedback mechanisms, to outline strategies to mitigate Arctic warming and to develop Nordic Earth System modelling with a focus on the short-lived climate forcers (SLCF), including natural and anthropogenic aerosols. The outcome of CRAICC is reflected in more than 150 peer-reviewed scientific publications, most of which are in the CRAICC special-issue of the journal Atmospheric Chemistry and Physics. This manuscript presents an overview on the main scientific topics investigated in the Centre and provides the reader a state-of-the-art comprehensive summary of what has been achieved in CRAICC with links to the particular publications for further detail. Facing the vast amount of outcomes we are not claiming to cover all results from CRAICC in this manuscript but concentrate here on the main results which are related to the feedback loops in the climate change-cryosphere interaction scheme affecting the Arctic amplification. [ABSTRACT FROM AUTHOR]

Recently significant advances have been made in the collection, detection and characterization of ice nucleating particles (INPs). Ice nuclei are particles that facilitate the heterogeneous formation of ice within the atmospheric aerosol by lowering the free energy barrier to spontaneous nucleation and growth of ice from atmospheric water and/or vapor. The Frankfurt isostatic diffusion chamber (FRankfurt Ice nucleation Deposition freezinG Experiment: FRIDGE) is an INP collection and offline detection system that has become widely deployed and shows additional potential for ambient measurements. Since its initial development FRIDGE has gone through several iterations and improvements. Here we describe improvements that have been made in the collection and analysis techniques. We detail the uncertainties inherent in the measurement method and suggest a systematic method of error analysis for FRIDGE measurements. Thus what is presented herein should serve as a foundation for the dissemination of all current and future measurements using FRIDGE instrumentation. [ABSTRACT FROM AUTHOR]