skip to main content


Title: A Microfluidic Device for Automated High Throughput Detection of Ice Nucleation of Snomax®
Measurement of ice nucleation (IN) temperature of liquid solutions at sub-ambient temperatures has applications in atmospheric, water quality, food storage, protein crystallography and pharmaceutical sciences. Here we present details on the construction of a temperature-controlled microfluidic platform with multiple individually addressable temperature zones and on-chip temperature sensors for high-throughput IN studies in droplets. We developed, for the first time, automated droplet freezing detection methods in a microfluidic device, using a deep neural network (DNN) and a polarized optical method based on intensity thresholding to classify droplets without manual counting. This platform has potential applications in continuous monitoring of liquid samples consisting of aerosols to quantify their IN behavior, or in checking for contaminants in pure water. A case study of the two detection methods was performed using Snomax® (Snomax International, Englewood, CO, USA), an ideal ice nucleating particle (INP). Effects of aging and heat treatment of Snomax® were studied with Fourier transform infrared (FTIR) spectroscopy and a microfluidic platform to correlate secondary structure change of the IN protein in Snomax® to IN temperature. It was found that aging at room temperature had a mild impact on the ice nucleation ability but heat treatment at 95 °C had a more pronounced effect by reducing the ice nucleation onset temperature by more than 7 °C and flattening the overall frozen fraction curve. Results also demonstrated that our setup can generate droplets at a rate of about 1500/min and requires minimal human intervention for DNN classification.  more » « less
Award ID(s):
1801971
NSF-PAR ID:
10232176
Author(s) / Creator(s):
; ;
Date Published:
Journal Name:
Micromachines
Volume:
12
Issue:
3
ISSN:
2072-666X
Page Range / eLocation ID:
296
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. The on-set of ice nucleation in mixed-phase clouds determines cloud lifetime and their microphysical properties. In this work, we develop a novel method that differentiates the early and later transition phases of mixed-phase clouds, i.e., ice crystals are initially surrounded by supercooled liquid water droplets, then as they grow, pure ice segments are formed. Using this method, we examine the relationship between the macrophysical and microphysical properties of mixed-phase clouds. The results show that evolution of cloud macrophysical properties, represented by the increasing spatial ratio of regions containing ice crystals relative to the total in-cloud region (defined as ice spatial ratio), is positively correlated with the evolution of microphysical properties, represented by the increasing ice water content and decreasing liquid water content. The mass partition transition from liquid to ice becomes more significant during the later transition phase (i.e., transition phase 3) when pure ice cloud regions (ICRs) start to appear. Occurrence frequencies of cloud thermodynamic phases show significant transition from liquid to ice at a similar temperature (i.e., -17.5 °C) among three types of definitions of mixed-phase clouds based on ice mass fraction, ice number fraction, or ice spatial ratio. Aerosol indirect effects are quantified for different transition phases using number concentrations of aerosols greater than 100 nm or 500 nm (N>100 and N>500, respectively). N>500 shows stronger positive correlations with ice spatial ratios compared with N>100. This result indicates that larger aerosols potentially contain ice nucleating particles, which facilitate the formation of ice crystals in mixed-phase clouds. The impact of N>500 is also more significant on the earlier transition phase when ice crystals just start to appear compared with the later transition phase. The thermodynamic and dynamic conditions are quantified for each transition phase. The results show in-cloud turbulence as a main mechanism for both the initiation of ice nucleation and the maintenance of supercooled liquid water, while updrafts are important for the latter but not the former. Overall, these results illustrate the varying effects of aerosols, thermodynamics, and dynamics throughout cloud evolution based on this new method that categorizes cloud transition phases. 
    more » « less
  2. Hazardous atmospheric icing conditions occur at sub-zero temperatures when droplets come into contact with aircraft and freeze, degrading aircraft performance and handling, introducing bias into some of the vital measurements needed for aircraft operation (e.g., air speed). Nonetheless, government regulations allow certified aircraft to fly in limited icing environments. The capability of aircraft sensors to identify all hazardous icing environments is limited. To address the current challenges in aircraft icing detection and protection, we present herein a platform designed for in-flight testing of ice protection solutions and icing detection technologies. The recently developed Platform for Ice-accretion and Coatings Tests with Ultrasonic Readings (PICTUR) was evaluated using CFD simulations and installed on the National Research Council Canada (NRC) Convair-580 aircraft that has flown in icing conditions over North East USA, during February 2022. This aircraft is a flying laboratory, equipped with more than 40 sensors providing a comprehensive characterization of the flight environment including measurements of temperature, pressure, wind speed and direction, water droplet size and number distribution, and hydrometeor habits imagery. The flight tests of the platform included assessment of passive icephobic coatings as well as heat-assisted tests. Monitoring tools included visual high resolution, real-time inspection of the surface as well as detection of surface ice using NRC’s Ultrasonic Ice Accretion Sensors (UIAS). In this paper, we present the new platform and show some preliminary commissioning results of PICTUR, collected inflight under, predominantly, supercooled small droplets and supercooled large drops (SLD) icing conditions. The combination of the platform and the complementary sensors on the aircraft demonstrated an effective and unique technique for icing studies in a natural environment.

     
    more » « less
  3. 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.

     
    more » « less
  4. Abstract

    This study investigates the evolution of temperature and lifetime of evaporating, supercooled cloud droplets considering initial droplet radius (r0) and temperature (), and environmental relative humidity (RH), temperature (T), and pressure (P). The time (tss) required by droplets to reach a lower steady-state temperature (Tss) after sudden introduction into a new subsaturated environment, the magnitude of ΔT=TTss, and droplet survival time (tst) atTssare calculated. The temperature difference (ΔT) is found to increase withT, and decrease with RH andP. ΔTwas typically 1–5 K lower thanT, with highest values (∼10.3 K) for very low RH, lowP, andTcloser to 0°C. Results show thattssis <0.5 s over the range of initial droplet and environmental conditions considered. Larger droplets (r0= 30–50μm) can survive atTssfor 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.Tssof 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. UsingTssinstead ofTin 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, andTcloser 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
  5. The formation of subcritical methanol clusters in the vapor phase is known to complicate the analysis of nucleation measurements. Here, we investigate how this process affects the onset of binary nucleation as dilute water–methanol mixtures in nitrogen carrier gas expand in a supersonic nozzle. These are the first reported data for water–methanol nucleation in an expansion device. We start by extending an older monomer–dimer–tetramer equilibrium model to include larger clusters, relying on Helmholtz free energy differences derived from Monte Carlo simulations. The model is validated against the pressure/temperature measurements of Laksmono et al. [Phys. Chem. Chem. Phys. 13, 5855 (2011)] for dilute methanol–nitrogen mixtures expanding in a supersonic flow prior to the appearance of liquid droplets. These data are well fit when the maximum cluster size imax is 6–12. The extended equilibrium model is then used to analyze the current data. On the addition of small amounts of water, heat release prior to particle formation is essentially unchanged from that for pure methanol, but liquid formation proceeds at much higher temperatures. Once water comprises more than ∼24 mol % of the condensable vapor, droplet formation begins at temperatures too high for heat release from subcritical cluster formation to perturb the flow. Comparing the experimental results to binary nucleation theory is challenged by the need to extrapolate data to the subcooled region and by the inapplicability of explicit cluster models that require a minimum of 12 molecules in the critical cluster. 
    more » « less