Abstract. Heterogeneous ice nucleation is thought to be the primary pathway for the formation of ice in mixed-phase clouds, with the number of active ice-nucleating particles (INPs) increasing rapidly with decreasing temperature. Here, molecular-dynamics simulations of heterogeneous ice nucleation demonstrate that the ice nucleation rate is also sensitive to pressure and that negative pressure within supercooled water shifts freezing temperatures to higher temperatures. Negative pressure, or tension, occurs naturally in water capillary bridges and pores and can also result from water agitation. Capillary bridge simulations presented in this study confirm that negative Laplace pressure within the water increases heterogeneous-freezing temperatures. The increase in freezing temperatures with negative pressure is approximately linear within the atmospherically relevant range of 1 to −1000 atm. An equation describing the slope depends on the latent heat of freezing and the molar volume difference between liquid water and ice. Results indicate that negative pressures of −500 atm, which correspond to nanometer-scale water surface curvatures, lead to a roughly 4 K increase in heterogeneous-freezing temperatures. In mixed-phase clouds, this would result in an increase of approximately 1 order of magnitude in active INP concentrations. The findings presented here indicate that any process leading to negative pressure in supercooled water may play a role in ice formation, consistent with experimental evidence of enhanced ice nucleation due to surface geometry or mechanical agitation of water droplets. This points towards the potential for dynamic processes such as contact nucleation and droplet collision or breakup to increase ice nucleation rates through pressure perturbations.
Ice-nucleation active (INA) bacteria can promote the growth of ice more effectively than any other known material. Using specialized ice-nucleating proteins (INPs), they obtain nutrients from plants by inducing frost damage and, when airborne in the atmosphere, they drive ice nucleation within clouds, which may affect global precipitation patterns. Despite their evident environmental importance, the molecular mechanisms behind INP-induced freezing have remained largely elusive. We investigate the structural basis for the interactions between water and the ice-nucleating protein InaZ from the INA bacterium
- NSF-PAR ID:
- 10214425
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 12
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
more » « less
-
more » « less
Abstract Here we report the ice nucleating temperatures of marine aerosols sampled in the subarctic Atlantic Ocean during a phytoplankton bloom. Ice nucleation measurements were conducted on primary aerosol samples and phytoplankton isolated from seawater samples. Primary marine aerosol samples produced by a specialized aerosol generator (the Sea Sweep) catalyzed droplet freezing at temperatures between −33.4 °C and − 24.5 °C, with a mean freezing temperature of −28.5 °C, which was significantly warmer than the homogeneous freezing temperature of pure water in the atmosphere (−36 °C). Following a storm‐induced deep mixing event, ice nucleation activity was enhanced by two metrics: (1) the fraction of aerosols acting as ice nucleating particles (INPs) and (2) the nucleating temperatures, which were the warmest observed throughout the project. Seawater samples were collected from the ocean's surface and phytoplankton groups, including
Synechococcus , picoeukaryotes, and nanoeukaryotes, were isolated into sodium chloride sheath fluid solution using a cell‐sorting flow cytometer. Marine aerosol containingSynechococcus , picoeukaryotes, and nanoeukaryotes serves as INP at temperatures significantly warmer than the homogeneous freezing temperature of pure water in the atmosphere. Samples containing whole organisms in 30 g L−1NaCl had freezing temperatures between −33.8 and − 31.1 °C. Dilution of samples to representative atmospheric aerosol salt concentrations (as low as 3.75 g L−1NaCl) raised freezing temperatures to as high as −22.1 °C. It follows that marine aerosols containing phytoplankton may have widespread influence on marine ice nucleation events by facilitating ice nucleation. -
more » « less
Abstract This study investigates the evolution of temperature and lifetime of evaporating, supercooled cloud droplets considering initial droplet radius (
r 0) and temperature (), and environmental relative humidity (RH), temperature ( T ∞), and pressure (P ). The time (t ss) required by droplets to reach a lower steady-state temperature (T ss) after sudden introduction into a new subsaturated environment, the magnitude of ΔT =T ∞−T ss, and droplet survival time (t st) atT ssare calculated. The temperature difference (ΔT ) is found to increase withT ∞, and decrease with RH andP . ΔT was typically 1–5 K lower thanT ∞, with highest values (∼10.3 K) for very low RH, lowP , andT ∞closer to 0°C. Results show thatt ssis <0.5 s over the range of initial droplet and environmental conditions considered. Larger droplets (r 0= 30–50μ m) can survive atT ssfor about 5 s to over 10 min, depending on the subsaturation of the environment. For higher RH and larger droplets, droplet lifetimes can increase by more than 100 s compared to those with droplet cooling ignored.T ssof the evaporating droplets can be approximated by the environmental thermodynamic wet-bulb temperature. Radiation was found to play a minor role in influencing droplet temperatures, except for larger droplets in environments close to saturation. The implications for ice nucleation in cloud-top generating cells and near cloud edges are discussed. UsingT ssinstead ofT ∞in widely used parameterization schemes could lead to enhanced number concentrations of activated ice-nucleating particles (INPs), by a typical factor of 2–30, with the greatest increases (≥100) coincident with low RH, lowP , andT ∞closer to 0°C.Significance Statement Cloud droplet temperature plays an important role in fundamental cloud processes like droplet growth and decay, activation of ice-nucleating particles, and determination of radiative parameters like refractive indices of water droplets. Near cloud boundaries such as cloud tops, dry air mixes with cloudy air exposing droplets to environments with low relative humidities. This study examines how the temperature of a cloud droplet that is supercooled (i.e., has an initial temperature < 0°C) evolves in these subsaturated environments. Results show that when supercooled cloud droplets evaporate near cloud boundaries, their temperatures can be several degrees Celsius lower than the surrounding drier environment. The implications of this additional cooling of droplets near cloud edges on ice particle formation are discussed.
-
more » « less
Abstract The abundance and sources of ice‐nucleating particles, particles required for heterogeneous ice nucleation, are long‐standing sources of uncertainty in quantifying aerosol‐cloud interactions. In this study, we demonstrate near closure between immersion freezing ice‐nucleating particle number concentration (
n INPs ) observations andn INPs calculated from simulated sea spray aerosol and dust. The Community Atmospheric Model with constrained meteorology was used to simulate aerosol concentrations at the Mace Head Research Station (North Atlantic) and over the Southern Ocean to the south of Tasmania (Clouds, Aerosols, Precipitation, Radiation, and atmospherIc Composition Over the southeRN ocean campaign). Model‐predictedn INPs were within a factor of 10 ofn INPs observed with an off‐line ice spectrometer at Mace Head Research Station and Clouds, Aerosols, Precipitation, Radiation, and atmospherIc Composition Over the southeRN ocean campaign, for 93% and 69% of observations, respectively. Simulated vertical profiles ofn INPs reveal that transported dust may be critical ton INPs in remote regions and that sea spray aerosol may be the dominate contributor to primary ice nucleation in Southern Ocean low‐level mixed‐phase clouds. -
more » « less
Ice nucleation and the resulting cloud glaciation are significant atmospheric processes that affect the evolution of clouds and their properties including radiative forcing and precipitation, yet the sources and properties of atmospheric ice nucleants are poorly constrained. Heterogeneous ice nucleation caused by ice-nucleating particles (INPs) enables cloud glaciation at temperatures above the homogeneous freezing regime that starts near −35 °C. Biomass burning is a significant global source of atmospheric particles and a highly variable and poorly understood source of INPs. The nature of these INPs and how they relate to the fuel composition and its combustion are critical gaps in our understanding of the effects of biomass burning on the environment and climate. Here we show that the combustion process transforms inorganic elements naturally present in the biomass (not soil or dust) to form potentially ice-active minerals in both the bottom ash and emitted aerosol particles. These particles possess ice-nucleation activities high enough to be relevant to mixed-phase clouds and are active over a wide temperature range, nucleating ice at up to −13 °C. Certain inorganic elements can thus serve as indicators to predict the production of ice nucleants from the fuel. Combustion-derived minerals are an important but understudied source of INPs in natural biomass-burning aerosol emissions in addition to lofted primary soil and dust particles. These discoveries and insights should advance the realistic incorporation of biomass-burning INPs into atmospheric cloud and climate models. These mineral components produced in biomass-burning aerosol should also be studied in relation to other atmospheric chemistry processes, such as facilitating multiphase chemical reactions and nutrient availability.
