Homogeneous Ice Nucleation in Subtropical and Tropical Convection and Its Influence on Cirrus Anvil Microphysics

2005 ◽  
Vol 62 (1) ◽  
pp. 41-64 ◽  
Author(s):  
Andrew J. Heymsfield ◽  
Larry M. Miloshevich ◽  
Carl Schmitt ◽  
Aaron Bansemer ◽  
Cynthia Twohy ◽  
...  

Abstract This study uses a unique set of microphysical measurements obtained in a vigorous, convective updraft core at temperatures between −33° and −36°C, together with a microphysical model, to investigate the role of homogeneous ice nucleation in deep tropical convection and how it influences the microphysical properties of the associated cirrus anvils. The core and anvil formed along a sea-breeze front during the Cirrus Regional Study of Tropical Anvils and Cirrus Layers–Florida Area Cirrus Experiment (CRYSTAL–FACE). The updraft core contained two distinct regions as traversed horizontally: the upwind portion of the core contained droplets of diameter 10–20 μm in concentrations of around 100 cm−3 with updraft speeds of 5–10 m s−1; the downwind portion of the core was glaciated with high concentrations of small ice particles and stronger updrafts of 10–20 m s−1. Throughout the core, rimed particles up to 0.6-cm diameter were observed. The anvil contained high concentrations of both small particles and large aggregates. Thermodynamic analysis suggests that the air sampled in the updraft core was mixed with air from higher altitudes that descended along the upwind edge of the cloud in an evaporatively driven downdraft, introducing free-tropospheric cloud condensation nuclei into the updraft below the aircraft sampling height. Farther downwind in the glaciated portion of the core, the entrained air contained high concentrations of ice particles that inhibit droplet formation and homogeneous nucleation. Calculations of droplet and ice particle growth and homogeneous ice nucleation are used to investigate the influence of large ice particles lofted in updrafts from lower levels in this and previously studied tropical ice clouds on the homogeneous nucleation process. The preexisting large ice particles act to suppress homogeneous nucleation through competition via diffusional and accretional growth, mainly when the updrafts are < 5 m s−1. In deep convective updrafts > 5–10 m s−1, the anvil is the depository for the small, radiatively important ice particles (homogeneously nucleated) and the large ice particles from below (heterogeneously or secondarily produced, or recycled).

2009 ◽  
Vol 66 (12) ◽  
pp. 3530-3562 ◽  
Author(s):  
Andrew J. Heymsfield ◽  
Aaron Bansemer ◽  
Gerald Heymsfield ◽  
Alexandre O. Fierro

Abstract Anvils produced by vigorous tropical convection contribute significantly to the earth’s radiation balance, and their radiative properties depend largely on the concentrations and sizes of the ice particles that form them. These microphysical properties are determined to an important extent by the fate of supercooled droplets, with diameters from 3 to about 20 microns, lofted in the updrafts. The present study addresses the question of whether most or all of these droplets are captured by ice particles or if they remain uncollected until arriving at the −38°C level where they freeze by homogeneous nucleation, producing high concentrations of very small ice particles that can persist and dominate the albedo. Aircraft data of ice particle and water droplet size distributions from seven field campaigns at latitudes from 25°N to 11°S are combined with a numerical model in order to examine the conditions under which significant numbers of supercooled water droplets can be lofted to the homogeneous nucleation level. Microphysical data were collected in pristine to heavily dust-laden maritime environments, isolated convective updrafts, and tropical cyclone updrafts with peak velocities reaching 25 m s−1. The cumulative horizontal distance of in-cloud sampling at temperatures of −20°C and below exceeds 50 000 km. Analysis reveals that most of the condensate in these convective updrafts is removed before reaching the −20°C level, and the total condensate continues to diminish linearly upward. The amount of condensate in small (<50 μm in diameter) droplets and ice particles, however, increases upward, suggesting new droplet activation with an appreciable radiative impact. Conditions promoting the generation of large numbers of small ice particles through homogeneous ice nucleation include high concentrations of cloud condensation nuclei (sometimes from dust), removal of most of the water substance between cloud base and the −38°C levels, and acceleration of the updrafts at mid- and upper levels such that velocities exceed 5–7 m s−1.


2006 ◽  
Vol 63 (7) ◽  
pp. 1752-1775 ◽  
Author(s):  
Susan C. van den Heever ◽  
Gustavo G. Carrió ◽  
William R. Cotton ◽  
Paul J. DeMott ◽  
Anthony J. Prenni

Abstract Toward the end of the Cirrus Regional Study of Tropical Anvils and Cirrus Layer–Florida Area Cirrus Experiment (CRYSTAL–FACE) field campaign held during July 2002, high concentrations of Saharan dust, which can serve as cloud condensation nuclei (CCN), giant CCN (GCCN), and ice-forming nuclei (IFN) were observed over the peninsula of Florida. To investigate the impacts of enhanced aerosol concentrations on the characteristics of convective storms and their subsequent anvil development, sensitivity tests are conducted using the Regional Atmospheric Modeling System (RAMS) model, in which the initialization profiles of CCN, GCCN, and IFN concentrations are varied. These variations are found to have significant effects on the storm dynamics and microphysical processes, as well as on the surface precipitation. Updrafts are consistently stronger as the aerosol concentrations are increased. The anvils cover a smaller area but are better organized and have larger condensate mixing ratio maxima in the cases with greater aerosol concentrations. Cloud water mass tends to increase with increasing aerosol concentrations, with enhanced GCCN concentrations having the most significant influence. Increasing either the GCCN or IFN concentrations produces the most rainfall at the surface whereas enhanced CCN concentrations reduce surface rainfall. Higher IFN concentrations produce ice at warmer temperatures and deeper anvils, but simultaneously increasing the concentrations of CCN and GCCN leads to more supercooled liquid water available for freezing and greater ice mixing ratios. Graupel mixing ratios decrease and hail mixing ratios increase with increasing aerosol concentrations. Higher concentrations of GCCN and IFN result in greater accumulated surface precipitation initially. By the end of the simulation period, however, the accumulated precipitation is the greatest for the case in which the aerosol concentrations are lowest. Such changes in the dynamical and microphysical characteristics of convective storms as a result of the variations in aerosol concentrations have potential climate consequences, both through cloud radiative effects and the hydrological cycle. The impacts of varying CCN, GCCN, and IFN concentrations on the anvils will be discussed more fully in Part II.


2006 ◽  
Vol 63 (1) ◽  
pp. 288-308 ◽  
Author(s):  
Andrew J. Heymsfield ◽  
Aaron Bansemer ◽  
Stephen L. Durden ◽  
Robert L. Herman ◽  
T. Paul Bui

Abstract Measurements are presented that were acquired from the National Aeronautics and Space Administration (NASA) DC-8 aircraft during an intensive 3-day study of Tropical Storm/Hurricane Humberto on 22, 23, and 24 September 2001. Particle size distributions, particle image information, vertical velocities, and single- and dual-wavelength Doppler radar observations were obtained during repeated sampling of the eyewall and outer eye regions. Eyewall sampling temperatures ranged from −22° to −57°C and peak updraft velocities from 4 to 15 m s−1. High concentrations of small ice particles, in the order 50 cm−3 and above, were observed within and around the updrafts. Aggregates, some larger than 7 mm, dominated the larger sizes. The slope of the fitted exponential size distributions λ was distinctly different close to the eye than outside of that region. Even at low temperatures, λ was characteristic of warm temperature growth (λ < 30 cm−1) close to the eye and characteristic of low temperature growth outside of it as well (λ > 100 cm−1). The two modes found for λ are shown to be consistent with observations from nonhurricane ice cloud layers formed through deep convection, but differ markedly from ice cloud layers generated in situ. It is shown that the median, mass-weighted, terminal velocities derived for the Humberto data and from the other datasets are primarily a function of λ. Microphysical measurements and dual wavelength radar observations are used together to infer and interpret particle growth processes. Rain in the lower portions of the eyewall extended up to the 6- or 7-km level. In the outer eye regions, aggregation progressed downward from between 8.5 and 11.9 km to the melting layer, with some graupel noted in rainbands. Homogeneous ice nucleation is implicated in the high concentrations of small ice particles observed in the vicinity of the updrafts.


2020 ◽  
Vol 20 (16) ◽  
pp. 10029-10045 ◽  
Author(s):  
James Brean ◽  
David C. S. Beddows ◽  
Zongbo Shi ◽  
Brice Temime-Roussel ◽  
Nicolas Marchand ◽  
...  

Abstract. Atmospheric aerosols contribute some of the greatest uncertainties to estimates of global radiative forcing and have significant effects on human health. New particle formation (NPF) is the process by which new aerosols of sub-2 nm diameter form from gas-phase precursors and contributes significantly to particle numbers in the atmosphere, accounting for approximately 50 % of cloud condensation nuclei globally. Here, we study summertime NPF in urban Barcelona in north-eastern Spain utilising particle counting instruments down to 1.9 nm and a Nitrate Chemical Ionisation Atmospheric Pressure interface Time of Flight Mass Spectrometer (CI-APi-ToF). The rate of formation of new particles is seen to increase linearly with sulfuric acid concentration, although particle formation rates fall short of chamber studies of H2SO4–DMA–H2O while exceeding those of H2SO4–BioOxOrg–H2O nucleation, although a role of highly oxygenated molecules (HOMs) cannot be ruled out. The sulfuric acid dimer : monomer ratio is significantly lower than that seen in experiments involving sulfuric acid and dimethylamine (DMA) in chambers, indicating that stabilisation of sulfuric acid clusters by bases is weaker in this dataset than in chambers, either due to rapid evaporation due to high summertime temperatures or limited pools of stabilising amines. Such a mechanism cannot be verified in these data, as no higher-order H2SO4–amine clusters nor H2SO4–HOM clusters were measured. The high concentrations of HOMs arise from isoprene, alkylbenzene, monoterpene and polycyclic aromatic hydrocarbon (PAH) oxidation, with alkylbenzenes providing greater concentrations of HOMs due to significant local sources. The concentration of these HOMs shows a dependence on temperature. The organic compounds measured primarily fall into the semivolatile organic compound (SVOC) volatility class arising from alkylbenzene and isoprene oxidation. Low-volatility organic compounds (LVOCs) largely arise from oxidation of alkylbenzenes, PAHs and monoterpenes, whereas extremely low-volatility organic compounds (ELVOCs) arise from primarily PAH and monoterpene oxidation. New particle formation without growth past 10 nm is also observed, and on these days oxygenated organic concentrations are lower than on days with growth by a factor of 1.6, and thus high concentrations of low-volatility oxygenated organics which primarily derive from traffic-emitted volatile organic compounds (VOCs) appear to be a necessary condition for the growth of newly formed particles in Barcelona. These results are consistent with prior observations of new particle formation from sulfuric acid–amine reactions in both chambers and the real atmosphere and are likely representative of the urban background of many European Mediterranean cities. A role for HOMs in the nucleation process cannot be confirmed or ruled out, and there is strong circumstantial evidence of the participation of HOMs across multiple volatility classes in particle growth.


Author(s):  
P.P.K. Smith

Grains of pigeonite, a calcium-poor silicate mineral of the pyroxene group, from the Whin Sill dolerite have been ion-thinned and examined by TEM. The pigeonite is strongly zoned chemically from the composition Wo8En64FS28 in the core to Wo13En34FS53 at the rim. Two phase transformations have occurred during the cooling of this pigeonite:- exsolution of augite, a more calcic pyroxene, and inversion of the pigeonite from the high- temperature C face-centred form to the low-temperature primitive form, with the formation of antiphase boundaries (APB's). Different sequences of these exsolution and inversion reactions, together with different nucleation mechanisms of the augite, have created three distinct microstructures depending on the position in the grain.In the core of the grains small platelets of augite about 0.02μm thick have farmed parallel to the (001) plane (Fig. 1). These are thought to have exsolved by homogeneous nucleation. Subsequently the inversion of the pigeonite has led to the creation of APB's.


2021 ◽  
Author(s):  
Erik H. Hoffmann ◽  
Andreas Tilgner ◽  
Simonas Kecorius ◽  
Hartmut Herrmann

<p>New particle formation (NPF) and early growth are efficient processes producing high concentrations of cloud condensation nuclei (CCNs) precursors in the Arctic marine boundary layer (AMBL). However, due to short lifetime and lack of condensable vapors, newly formed particles do often not grow beyond 50 nm and cause low CCN particle concentrations in the AMBL. Thus, even the smallest amount of Aitken mode particle growth is capable to significantly increase the CCN budget. However, the growth mechanism of Aitken-mode particles from NPF into CCN range in the Arctic is still rather unclear and was therefore investigated during the cruise campaign PASCAL in 2017.</p> <p>During PASCAL, aerosol particles measurements were performed and an unexpected rapid growth of Aitken mode particles was observed right after fog episodes. Combined field data analyses and detailed multiphase chemistry box model simulations with the CAPRAM mechanism were performed to study the underlying processes. Resulting, a new mechanism is proposed explaining how particles with d < 50 nm are able to grow into CCN size range in the Arctic without requiring high water vapor supersaturation (SS). The investigations demonstrated that the rapid post-fog particle growth of Aitken mode is related to chemical processes within the Arctic fog. The redistribution of semi-volatile acidic (e.g., methanesulfonic acid) and basic (e.g., ammonia) compounds from processed CCN-active particles to smaller CCN-inactive particles can cause a rapid particle growth of Aitken mode particles after fog evaporation enabling them to grow towards CCN size. Comparisons of the model results with Berner impactor measurements supports the proposed growth mechanism.</p> <p>Overall, this study provided new insights on how the increasing frequency of NPF and fog-related particle processing can increase in the number of CCNs and cloud droplets leading to an increased albedo of Arctic clouds and thus affect the radiative balance in the Arctic. Since fogs will occur more frequently in the Arctic as a result of climate change, this growth mechanism and a deeper knowledge on its feedbacks can be essential to understand Arctic warming.</p>


Author(s):  
Alexander Bucknell ◽  
Matthew McGilvray ◽  
David R. H. Gillespie ◽  
Geoff Jones ◽  
Alasdair Reed ◽  
...  

It has been recognised in recent years that high altitude atmospheric ice crystals pose a threat to aircraft engines. Instances of damage, surge and shutdown have been recorded at altitudes significantly greater than those associated with supercooled water icing. It is believed that solid ice particles can accrete inside the core compressor, although the exact mechanism by which this occurs remains poorly understood. Development of analytical and empirical models of the ice crystal icing phenomenon is necessary for both future engine design and this-generation engine certification. A comprehensive model will require the integration of a number of aerodynamic, thermodynamic and mechanical components. This paper studies one such component, specifically the thermodynamic and mechanical processes experienced by ice particles impinging on a warm surface. Results are presented from an experimental campaign using a heated and instrumented flat plate. The plate was installed in the Altitude Icing Wind Tunnel (AIWT) at the National Research Council of Canada (NRC). This facility is capable of replicating ice crystal conditions at altitudes up to 9 km and Mach numbers up to 0.55 [1]. The heated plate is designed to measure the heat flux from a surface at temperatures representative of the early core compressor, under varying convective and icing heat loads. Heat transfer enhancement was observed to rise approximately linearly with both total water content and particle diameter over the ranges tested. A Stokes number greater than unity proved to be a useful parameter in determining whether heat transfer enhancement would occur. A particle energy parameter was used to estimate the likelihood of fragmentation. Results showed that when particles were both ballistic and likely to fragment, heat transfer enhancement was independent of both Mach and Reynolds numbers over the ranges tested.


2011 ◽  
Vol 11 (11) ◽  
pp. 5289-5303 ◽  
Author(s):  
G. Grell ◽  
S. R. Freitas ◽  
M. Stuefer ◽  
J. Fast

Abstract. A plume rise algorithm for wildfires was included in WRF-Chem, and applied to look at the impact of intense wildfires during the 2004 Alaska wildfire season on weather simulations using model resolutions of 10 km and 2 km. Biomass burning emissions were estimated using a biomass burning emissions model. In addition, a 1-D, time-dependent cloud model was used online in WRF-Chem to estimate injection heights as well as the vertical distribution of the emission rates. It was shown that with the inclusion of the intense wildfires of the 2004 fire season in the model simulations, the interaction of the aerosols with the atmospheric radiation led to significant modifications of vertical profiles of temperature and moisture in cloud-free areas. On the other hand, when clouds were present, the high concentrations of fine aerosol (PM2.5) and the resulting large numbers of Cloud Condensation Nuclei (CCN) had a strong impact on clouds and cloud microphysics, with decreased precipitation coverage and precipitation amounts during the first 12 h of the integration. During the afternoon, storms were of convective nature and appeared significantly stronger, probably as a result of both the interaction of aerosols with radiation (through an increase in CAPE) as well as the interaction with cloud microphysics.


2020 ◽  
Vol 13 (9) ◽  
pp. 4107-4157 ◽  
Author(s):  
Shin-ichiro Shima ◽  
Yousuke Sato ◽  
Akihiro Hashimoto ◽  
Ryohei Misumi

Abstract. The super-droplet method (SDM) is a particle-based numerical scheme that enables accurate cloud microphysics simulation with lower computational demand than multi-dimensional bin schemes. Using SDM, a detailed numerical model of mixed-phase clouds is developed in which ice morphologies are explicitly predicted without assuming ice categories or mass–dimension relationships. Ice particles are approximated using porous spheroids. The elementary cloud microphysics processes considered are advection and sedimentation; immersion/condensation and homogeneous freezing; melting; condensation and evaporation including cloud condensation nuclei activation and deactivation; deposition and sublimation; and coalescence, riming, and aggregation. To evaluate the model's performance, a 2-D large-eddy simulation of a cumulonimbus was conducted, and the life cycle of a cumulonimbus typically observed in nature was successfully reproduced. The mass–dimension and velocity–dimension relationships the model predicted show a reasonable agreement with existing formulas. Numerical convergence is achieved at a super-particle number concentration as low as 128 per cell, which consumes 30 times more computational time than a two-moment bulk model. Although the model still has room for improvement, these results strongly support the efficacy of the particle-based modeling methodology to simulate mixed-phase clouds.


2012 ◽  
Vol 12 (1) ◽  
pp. 623-689 ◽  
Author(s):  
G. W. Mann ◽  
K. S. Carslaw ◽  
D. A. Ridley ◽  
D. V. Spracklen ◽  
K. J. Pringle ◽  
...  

Abstract. A global modal aerosol microphysics module (GLOMAP-mode) is evaluated and improved by comparing against a sectional version (GLOMAP-bin) and observations in the same 3-D global offline chemistry transport model. With both schemes, the model captures the main features of the global particle size distribution, with sub-micron aerosol approximately unimodal in continental regions and bi-modal in marine regions. Initial bin-mode comparisons showed that various size distribution parameter settings (mode widths and inter-modal separation sizes) resulted in clear biases compared to the sectional scheme. By adjusting these parameters in the modal scheme, much better agreement is achieved against the bin scheme and observations. Surface mass of sulphate, sea-salt, black carbon (BC) and organic carbon (OC) are, on the annual mean, within 25 % in the two schemes in nearly all regions. On the annual mean, surface level concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), surface area density and condensation sink also compare within 25 % in most regions. However, marine CCN concentrations between 30° N and 30° S are systematically higher in the modal scheme, by 25–60 %, which we attribute to differences in size-resolved particle growth or cloud-processing. Larger differences also exist in regions or seasons dominated by biomass burning and in free-troposphere and high-latitude regions. Indeed, in the free-troposphere, GLOMAP-mode BC is a factor 2–4 higher than GLOMAP-bin, likely due to differences in size-resolved scavenging. Nevertheless, in most parts of the atmosphere, we conclude that bin-mode differences are much less than model-observation differences, although some processes are missing in these runs which may pose a bigger challenge to modal schemes (e.g. boundary layer nucleation, ultra-fine sea-spray). The findings here underline the need for a spectrum of complexity in global models, with size-resolved aerosol properties predicted by modal schemes needing to be continually benchmarked and improved against freely evolving sectional schemes and observations.


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