scholarly journals The Portable Ice Nucleation Experiment (PINE): a new online instrument for laboratory studies and automated long-term field observations of ice-nucleating particles

2021 ◽  
Vol 14 (2) ◽  
pp. 1143-1166
Author(s):  
Ottmar Möhler ◽  
Michael Adams ◽  
Larissa Lacher ◽  
Franziska Vogel ◽  
Jens Nadolny ◽  
...  
Keyword(s):  
Pure Water ◽  
Full Range ◽  
Field Measurements ◽  
Ice Nucleation ◽  
Spatial And Temporal Variation ◽  
Expansion Chamber ◽  
Predictive Capacity ◽  
Field Campaign ◽  
New Instrument ◽  
Term Field

Abstract. Atmospheric ice-nucleating particles (INPs) play an important role in determining the phase of clouds, which affects their albedo and lifetime. A lack of data on the spatial and temporal variation of INPs around the globe limits our predictive capacity and understanding of clouds containing ice. Automated instrumentation that can robustly measure INP concentrations across the full range of tropospheric temperatures is needed in order to address this knowledge gap. In this study, we demonstrate the functionality and capacity of the new Portable Ice Nucleation Experiment (PINE) to study ice nucleation processes and to measure INP concentrations under conditions pertinent for mixed-phase clouds, with temperatures from about −10 to about −40 ∘C. PINE is a cloud expansion chamber which avoids frost formation on the cold walls and thereby omits frost fragmentation and related background ice signals during the operation. The development, working principle and treatment of data for the PINE instrument is discussed in detail. We present laboratory-based tests where PINE measurements were compared with those from the established AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber. Within experimental uncertainties, PINE agreed with AIDA for homogeneous freezing of pure water droplets and the immersion freezing activity of mineral aerosols. Results from a first field campaign conducted at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) observatory in Oklahoma, USA, from 1 October to 14 November 2019 with the latest PINE design (a commercially available PINE chamber) are also shown, demonstrating PINE's ability to make automated field measurements of INP concentrations at a time resolution of about 8 min with continuous temperature scans for INP measurements between −10 and −30 ∘C. During this field campaign, PINE was continuously operated for 45 d in a fully automated and semi-autonomous way, demonstrating the capability of this new instrument to also be used for longer-term field measurements and INP monitoring activities in observatories.

scholarly journals The portable ice nucleation experiment PINE: a new online instrument for laboratory studies and automated long-term field observations of ice-nucleating particles

2020 ◽  
Author(s):  
Ottmar Möhler ◽  
Michael Adams ◽  
Larissa Lacher ◽  
Franziska Vogel ◽  
Jens Nadolny ◽  
...  
Keyword(s):  
Pure Water ◽  
Full Range ◽  
Field Measurements ◽  
Ice Nucleation ◽  
Spatial And Temporal Variation ◽  
High Time Resolution ◽  
Expansion Chamber ◽  
Field Campaign ◽  
New Instrument ◽  
Term Field

Abstract. Atmospheric ice-nucleating particles (INP) play an important role in determining the phase of clouds, which affects their albedo and lifetime. A lack of data on the spatial and temporal variation of INPs around the globe limits our predictive capacity and understanding of clouds containing ice. Automated instrumentation that can robustly measure INP concentrations across the full range of tropospheric temperatures is needed in order to address this knowledge gap. In this study, we demonstrate the functionality and capacity of the new Portable Ice Nucleation Experiment (PINE) to study ice nucleation processes and to measure INP concentrations under conditions pertinent for mixed-phase clouds, with temperatures from about −10 °C to about −38 °C. PINE is a cloud expansion chamber which avoids frost formation on the cold walls, and thereby omits frost fragmentation and related background ice signals during the operation. The development, working principle, and treatment of data for the PINE instrument is discussed in detail. We present extensive laboratory based tests where PINE measurements were compared with those from the established AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber. The results show good agreement of PINE with AIDA for homogeneous freezing of pure water droplets and the immersion freezing activity of mineral aerosols. Results from a first field campaign conducted at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) observatory in Oklahoma, USA, from October 1 to November 14, 2019 with the latest PINE design (a commercially available PINE chamber) are also shown, demonstrating PINE’s ability to make automated field measurements of INP concentrations at high time resolution of about 8 minutes with continuous wall temperature scans between −5 and −35 °C. During this field campaign, PINE was continuously operated for 45 days in a fully automated and semi-autonomous way, demonstrating the capability of this new instrument to be also used for longer term field measurements and INP monitoring activities in observatories.

scholarly journals Measurements of OH and HO<sub>2</sub> concentrations during the MCMA-2006 field campaign – Part 1: Deployment of the Indiana University laser-induced fluorescence instrument

2008 ◽  
Vol 8 (4) ◽  
pp. 13689-13739 ◽  
Author(s):  
S. Dusanter ◽  
D. Vimal ◽  
P. S. Stevens ◽  
R. Volkamer ◽  
L. T. Molina
Keyword(s):  
Mexico City ◽  
Signal To Noise Ratio ◽  
Field Measurements ◽  
Laser Induced Fluorescence ◽  
Urban Site ◽  
Indiana University ◽  
Field Campaign ◽  
Direct Excitation ◽  
Stage Of Development ◽  
New Instrument

Abstract. Measurements of tropospheric hydroxyl (OH) and hydroperoxy (HO2) radicals were made during the MCMA (Mexico City Metropolitan Area) field campaign as part of the MILAGRO (Megacity Initiative: Local and Global Research Observations) project during March 2006. These radicals were measured using a laser-induced fluorescence instrument developed at Indiana University. This new instrument takes advantage of the Fluorescence Assay by Gas Expansion technique (FAGE) together with direct excitation and detection of OH at 308 nm. HO2 is indirectly measured as OH by titration with NO inside the fluorescence cell. At this stage of development, IU-FAGE is capable of detecting 3.9×105molec cm−3 of both OH and HO2, with a signal to noise ratio of 1, an averaged laser power of 10 mW and an averaging time of 5 min. The calibration accuracies (1σ) are ±17% for OH and ±18% for HO2 using the water-vapor photolysis/O2 actinometry calibration technique. OH and HO2 concentrations were successfully measured at an urban site in Mexico City, with observed concentrations comparable to those measured in other polluted environments. Enhanced levels of OH and HO2 radicals were observed on several days between 09:30–11 a.m. and suggest an intense photochemistry during morning hours that may be due to elevated sources of HOx (OH+HO2) and a fast cycling between the radicals under the high NOx conditions of the MCMA. A comparison with other urban and sub-urban field measurements suggests that OH concentrations are highly buffered under these conditions. In contrast, HO2 concentrations are highly variable between different urban sites.

scholarly journals Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions – Part 2: Quartz and amorphous silica

2019 ◽  
Vol 19 (9) ◽  
pp. 6035-6058 ◽  
Author(s):  
Anand Kumar ◽  
Claudia Marcolli ◽  
Thomas Peter
Keyword(s):  
Aqueous Solutions ◽  
Amorphous Silica ◽  
Pure Water ◽  
Ice Nucleation ◽  
Water Volume ◽  
Special Focus ◽  
Quartz Surface ◽  
Mineral Surface ◽  
Glass Vial ◽  
Immersion Freezing

Abstract. Divergent ice nucleation (IN) efficiencies of quartz, an important component of atmospheric mineral dust, have been reported in previous studies. We show here that quartz particles obtain their IN activity from milling and that quartz aged in water loses most of its IN efficiency relative to freshly milled quartz. Since most studies so far reported IN activities of commercial quartz dusts that were milled already by the manufacturer, IN active samples prevailed. Also, the quartz surface – much in contrast to that of feldspars – is not prone to ammonia-induced IN enhancement. In detail we investigate the influence of solutes on the IN efficiency of various silica (SiO2) particles (crystalline and amorphous) with special focus on quartz. We performed immersion freezing experiments and relate the observed variability in IN activity to the influence of milling, the aging time and to the exposure conditions since milling. Immersion freezing with silica particles suspended in pure water or aqueous solutions of NH3, (NH4)2SO4, NH4HSO4, Na2SO4 and NaOH, with solute concentrations corresponding to water activities aw=0.9–1.0, were investigated in emulsified droplets by means of differential scanning calorimetry (DSC) and analyzed in terms of the onset temperature of the heterogeneous freezing signal Thet and the heterogeneously frozen water volume fraction Fhet. Quartz particles, which originate from milling coarse samples, show a strong heterogeneous freezing peak in pure water with Thet equal to 247–251 K. This IN activity disappears almost completely after aging for 7 months in pure water in a glass vial. During this time quartz slowly grew by incorporating silicic acid leached from the glass vial. Conversely, the synthesized amorphous silica samples show no discernable heterogeneous freezing signal unless they were milled. This implies that defects provide IN activity to silica surfaces, whereas the IN activity of a natural quartz surface is negligible, when it grew under near-equilibrium conditions. For suspensions containing milled quartz and the solutes (NH4)2SO4, NH4HSO4 or Na2SO4, Thet approximately follows ThetΔawhet(aw), the heterogeneous freezing onset temperatures that obey Δawhet criterion, i.e., ThetΔawhet(aw)=Tmelt(aw+Δawhet) with Δawhet being a constant offset with respect to the ice melting point curve, similar to homogeneous IN. This water-activity-based description is expected to hold when the mineral surface is not altered by the presence of the solutes. On the other hand, we observe a slight enhancement in Fhet in the presence of these solutes, implying that the compliance with the Δawhet criterion does not necessarily imply constant Fhet. In contrast to the sulfates, dilute solutions of NH3 or NaOH (molality ≥5×10-4 mol kg−1) reveal Thet by 3–8 K lower than ThetΔawhet(aw), indicating a significant impact on the mineral surface. The lowering of Thet of quartz suspended in dilute NH3 solutions is opposite to the distinct increase in Thet that we found in emulsion freezing experiments with aluminosilicates, namely feldspars, kaolinite, gibbsite and micas. We ascribe this decrease in IN activity to the increased dissolution of quartz under alkaline conditions. The defects that constitute the active sites appear to be more susceptible to dissolution and therefore disappear first on a dissolving surface.

Freezing of micrometer-sized liquid droplets of pure water evaporatively cooled in a vacuum

2018 ◽  
Vol 20 (45) ◽  
pp. 28435-28444 ◽  
Author(s):  
Kota Ando ◽  
Masashi Arakawa ◽  
Akira Terasaki
Keyword(s):  
Pure Water ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Liquid Droplets ◽  
Freezing Time ◽  
Water Droplets

The freezing time of pure-water droplets is measured in a vacuum and simulated by ice nucleation theory.

scholarly journals Cleaning up our water: reducing interferences from nonhomogeneous freezing of “pure” water in droplet freezing assays of ice-nucleating particles

2018 ◽  
Vol 11 (9) ◽  
pp. 5315-5334 ◽  
Author(s):  
Michael Polen ◽  
Thomas Brubaker ◽  
Joshua Somers ◽  
Ryan C. Sullivan
Keyword(s):  
Pure Water ◽  
Freezing Temperature ◽  
Cloud Microphysics ◽  
Ice Nucleation ◽  
Great Promise ◽  
Water Control ◽  
Temperature Spectra ◽  
Droplet Sizes ◽  
Mixed Phase Clouds ◽  
Insight Into

Abstract. Droplet freezing techniques (DFTs) have been used for half a century to measure the concentration of ice-nucleating particles (INPs) in the atmosphere and determine their freezing properties to understand the effects of INPs on mixed-phase clouds. The ice nucleation community has recently adopted droplet freezing assays as a commonplace experimental approach. These droplet freezing experiments are often limited by contamination that causes nonhomogeneous freezing of the “pure” water used to generate the droplets in the heterogeneous freezing temperature regime that is being measured. Interference from the early freezing of water is often overlooked and not fully reported, or measurements are restricted to analyzing the more ice-active INPs that freeze well above the temperature of the background water. However, this avoidance is not viable for analyzing the freezing behavior of less active INPs in the atmosphere that still have potentially important effects on cold-cloud microphysics. In this work we review a number of recent droplet freezing techniques that show great promise in reducing these interferences, and we report our own extensive series of measurements using similar methodologies. By characterizing the performance of different substrates on which the droplets are placed and of different pure water generation techniques, we recommend best practices to reduce these interferences. We tested different substrates, water sources, droplet matrixes, and droplet sizes to provide deeper insight into what methodologies are best suited for DFTs. Approaches for analyzing droplet freezing temperature spectra and accounting and correcting for the background “pure” water control spectrum are also presented. Finally, we propose experimental and data analysis procedures for future homogeneous and heterogeneous ice nucleation studies to promote a more uniform and reliable methodology that facilitates the ready intercomparison of ice-nucleating particles measured by DFTs.

scholarly journals Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions. Part 2 – Quartz and amorphous silica

2018 ◽  
Author(s):  
Anand Kumar ◽  
Claudia Marcolli ◽  
Thomas Peter
Keyword(s):  
Aqueous Solutions ◽  
Amorphous Silica ◽  
Pure Water ◽  
Ice Nucleation ◽  
Water Volume ◽  
Special Focus ◽  
Quartz Surface ◽  
Mineral Surface ◽  
Glass Vial ◽  
Immersion Freezing

Abstract. Divergent ice nucleation (IN) efficiencies of quartz, an important component of atmospheric mineral dust, have been reported in previous studies. We show here that quartz particles obtain their IN activity from milling and that quartz aged in water loses most of its IN efficiency relative to freshly milled quartz. Also, the quartz surface – much in contrast to that of feldspars – is not prone to ammonia-induced IN enhancement. In detail we investigate the influence of solutes on the IN efficiency of various silica (SiO2) particles (crystalline and amorphous) with special focus on quartz. We performed immersion freezing experiments and relate the reported contradictory behavior to the influence of milling, and to the aging time and conditions since milling. Immersion freezing with silica particles suspended in pure water or aqueous solutions of NH3, (NH4)2SO4, NH4HSO4, Na2SO4 and NaOH, with solute concentrations corresponding to water activities aw = 0.9–1.0, were investigated in emulsified droplets by means of differential scanning calorimetry (DSC) and analyzed in terms of the onset temperature of the heterogeneous freezing signal Thet and the heterogeneously frozen water volume fraction Fhet. Quartz particles, which originate from milling coarse samples, show a strong heterogeneous freezing peak in pure water with Thet = 247–251 K. This IN activity disappears almost completely after aging for 7 months in pure water in a glass vial. During this time quartz slowly grew by incorporating silicic acid leached from the glass vial. Conversely, the synthesized amorphous silica samples show no discernable heterogeneous freezing signal unless they were milled. This implies that defects provide IN activity to silica surfaces, whereas the IN activity of a natural quartz surface is negligible, when it grew under near-equilibrium conditions. For suspensions containing milled quartz and the solutes (NH4)2SO4, NH4HSO4 or Na2SO4, Thet approximately follows Thet(Δawhet) (aw), the heterogeneous freezing onset temperatures that obey Δawhet-criterion, i.e. Thet(Δawhet) (aw) = Tmelt (aw + Δawhet) with Δawhet being a constant offset with respect to the ice melting point curve, similar to homogeneous IN. This water-activity-based description is expected to hold when the mineral surface is not altered by the presence of the solutes. On the other hand, we observe a slight enhancement in Fhet in the presence of these solutes, implying that the compliance with the Δawhet-criterion does not necessarily imply constant Fhet. In contrast to the sulfates, dilute solutions of NH3 or NaOH (molality &amp;geq; 5 × 10−4 mol kg−1) reveal Thet by 3–8 K lower than Thet(Δawhet) (aw), indicating a significant impact on the mineral surface. The lowering of Thet of quartz suspended in dilute NH3 solutions is opposite to the distinct increase in Thet that we found in emulsion freezing experiments with aluminosilicates, namely feldspars, kaolinite, gibbsite and micas. We ascribe this decrease of IN activity to the increased dissolution of quartz under alkaline conditions. The defects that constitute the active sites appear to be more susceptible to dissolution and therefore disappear first on a dissolving surface.

scholarly journals Ice nucleation efficiency of clay minerals in the immersion mode

2012 ◽  
Vol 12 (13) ◽  
pp. 5859-5878 ◽  
Author(s):  
V. Pinti ◽  
C. Marcolli ◽  
B. Zobrist ◽  
C. R. Hoyle ◽  
T. Peter
Keyword(s):  
Clay Minerals ◽  
Clay Mineral ◽  
Differential Scanning Calorimeter ◽  
Pure Water ◽  
Nucleation Site ◽  
Ice Nucleation ◽  
Nucleation Sites ◽  
The One ◽  
Site Classes

Abstract. Emulsion and bulk freezing experiments were performed to investigate immersion ice nucleation on clay minerals in pure water, using various kaolinites, montmorillonites, illites as well as natural dust from the Hoggar Mountains in the Saharan region. Differential scanning calorimeter measurements were performed on three different kaolinites (KGa-1b, KGa-2 and K-SA), two illites (Illite NX and Illite SE) and four natural and acid-treated montmorillonites (SWy-2, STx-1b, KSF and K-10). The emulsion experiments provide information on the average freezing behaviour characterized by the average nucleation sites. These experiments revealed one to sometimes two distinct heterogeneous freezing peaks, which suggest the presence of a low number of qualitatively distinct average nucleation site classes. We refer to the peak at the lowest temperature as "standard peak" and to the one occurring in only some clay mineral types at higher temperatures as "special peak". Conversely, freezing in bulk samples is not initiated by the average nucleation sites, but by a very low number of "best sites". The kaolinites and montmorillonites showed quite narrow standard peaks with onset temperatures 238 K

scholarly journals The Horizontal Ice Nucleation Chamber (HINC): INP measurements at conditions relevant for mixed-phase clouds at the High Altitude Research Station Jungfraujoch

2017 ◽  
Vol 17 (24) ◽  
pp. 15199-15224 ◽  
Author(s):  
Larissa Lacher ◽  
Ulrike Lohmann ◽  
Yvonne Boose ◽  
Assaf Zipori ◽  
Erik Herrmann ◽  
...  
Keyword(s):  
High Altitude ◽  
Ice Nucleation ◽  
Mixed Phase ◽  
Saharan Dust ◽  
Research Station ◽  
Minimum Detectable Concentration ◽  
The North ◽  
New Instrument ◽  
Marine Air ◽  
Mixed Phase Clouds

Abstract. In this work we describe the Horizontal Ice Nucleation Chamber (HINC) as a new instrument to measure ambient ice-nucleating particle (INP) concentrations for conditions relevant to mixed-phase clouds. Laboratory verification and validation experiments confirm the accuracy of the thermodynamic conditions of temperature (T) and relative humidity (RH) in HINC with uncertainties in T of ±0.4 K and in RH with respect to water (RHw) of ±1.5 %, which translates into an uncertainty in RH with respect to ice (RHi) of ±3.0 % at T > 235 K. For further validation of HINC as a field instrument, two measurement campaigns were conducted in winters 2015 and 2016 at the High Altitude Research Station Jungfraujoch (JFJ; Switzerland, 3580 m a. s. l. ) to sample ambient INPs. During winters 2015 and 2016 the site encountered free-tropospheric conditions 92 and 79 % of the time, respectively. We measured INP concentrations at 242 K at water-subsaturated conditions (RHw = 94 %), relevant for the formation of ice clouds, and in the water-supersaturated regime (RHw = 104 %) to represent ice formation occurring under mixed-phase cloud conditions. In winters 2015 and 2016 the median INP concentrations at RHw = 94 % was below the minimum detectable concentration. At RHw = 104 %, INP concentrations were an order of magnitude higher, with median concentrations in winter 2015 of 2.8 per standard liter (std L−1; normalized to standard T of 273 K and pressure, p, of 1013 hPa) and 4.7 std L−1 in winter 2016. The measurements are in agreement with previous winter measurements obtained with the Portable Ice Nucleation Chamber (PINC) of 2.2 std L−1 at the same location. During winter 2015, two events caused the INP concentrations at RHw = 104 % to significantly increase above the campaign average. First, an increase to 72.1 std L−1 was measured during an event influenced by marine air, arriving at the JFJ from the North Sea and the Norwegian Sea. The contribution from anthropogenic or other sources can thereby not be ruled out. Second, INP concentrations up to 146.2 std L−1 were observed during a Saharan dust event. To our knowledge this is the first time that a clear enrichment in ambient INP concentration in remote regions of the atmosphere is observed during a time of marine air mass influence, suggesting the importance of marine particles on ice nucleation in the free troposphere.

scholarly journals Contribution of feldspar and marine organic aerosols to global ice nucleating particle concentrations

2017 ◽  
Vol 17 (5) ◽  
pp. 3637-3658 ◽  
Author(s):  
Jesús Vergara-Temprado ◽  
Benjamin J. Murray ◽  
Theodore W. Wilson ◽  
Daniel O'Sullivan ◽  
Jo Browse ◽  
...  
Keyword(s):  
Regional Distribution ◽  
Organic Aerosols ◽  
Field Measurements ◽  
Field Work ◽  
Ice Nucleation ◽  
Mixed Phase ◽  
Aerosol Composition ◽  
Desert Dust ◽  
Concentration Changes ◽  
Mixed Phase Clouds

Abstract. Ice-nucleating particles (INPs) are known to affect the amount of ice in mixed-phase clouds, thereby influencing many of their properties. The atmospheric INP concentration changes by orders of magnitude from terrestrial to marine environments, which typically contain much lower concentrations. Many modelling studies use parameterizations for heterogeneous ice nucleation and cloud ice processes that do not account for this difference because they were developed based on INP measurements made predominantly in terrestrial environments without considering the aerosol composition. Errors in the assumed INP concentration will influence the simulated amount of ice in mixed-phase clouds, leading to errors in top-of-atmosphere radiative flux and ultimately the climate sensitivity of the model. Here we develop a global model of INP concentrations relevant for mixed-phase clouds based on laboratory and field measurements of ice nucleation by K-feldspar (an ice-active component of desert dust) and marine organic aerosols (from sea spray). The simulated global distribution of INP concentrations based on these two species agrees much better with currently available ambient measurements than when INP concentrations are assumed to depend only on temperature or particle size. Underestimation of INP concentrations in some terrestrial locations may be due to the neglect of INPs from other terrestrial sources. Our model indicates that, on a monthly average basis, desert dusts dominate the contribution to the INP population over much of the world, but marine organics become increasingly important over remote oceans and they dominate over the Southern Ocean. However, day-to-day variability is important. Because desert dust aerosol tends to be sporadic, marine organic aerosols dominate the INP population on many days per month over much of the mid- and high-latitude Northern Hemisphere. This study advances our understanding of which aerosol species need to be included in order to adequately describe the global and regional distribution of INPs in models, which will guide ice nucleation researchers on where to focus future laboratory and field work.

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