scholarly journals Ice Initiation by Aerosol Particles: Measured and Predicted Ice Nuclei Concentrations versus Measured Ice Crystal Concentrations in an Orographic Wave Cloud

2010 ◽  
Vol 67 (8) ◽  
pp. 2417-2436 ◽  
Author(s):  
T. Eidhammer ◽  
P. J. DeMott ◽  
A. J. Prenni ◽  
M. D. Petters ◽  
C. H. Twohy ◽  
...  

Abstract The initiation of ice in an isolated orographic wave cloud was compared with expectations based on ice nucleating aerosol concentrations and with predictions from new ice nucleation parameterizations applied in a cloud parcel model. Measurements of ice crystal number concentrations were found to be in good agreement both with measured number concentrations of ice nuclei feeding the clouds and with ice nuclei number concentrations determined from the residual nuclei of cloud particles collected by a counterflow virtual impactor. Using lognormal distributions fitted to measured aerosol size distributions and measured aerosol chemical compositions, ice nuclei and ice crystal concentrations in the wave cloud were reasonably well predicted in a 1D parcel model framework. Two different empirical parameterizations were used in the parcel model: a parameterization based on aerosol chemical type and surface area and a parameterization that links ice nuclei number concentrations to the number concentrations of particles with diameters larger than 0.5 μm. This study shows that aerosol size distribution and composition measurements can be used to constrain ice initiation by primary nucleation in models. The data and model results also suggest the likelihood that the dust particle mode of the aerosol size distribution controls the number concentrations of the heterogeneous ice nuclei, at least for the lower temperatures examined in this case.

2012 ◽  
Vol 5 (3) ◽  
pp. 845-868 ◽  
Author(s):  
T. Bergman ◽  
V.-M. Kerminen ◽  
H. Korhonen ◽  
K. J. Lehtinen ◽  
R. Makkonen ◽  
...  

Abstract. We present the implementation and evaluation of a sectional aerosol microphysics module SALSA within the aerosol-climate model ECHAM5-HAM. This aerosol microphysics module has been designed to be flexible and computationally efficient so that it can be implemented in regional or global scale models. The computational efficiency has been achieved by minimising the number of variables needed to describe the size and composition distribution. The aerosol size distribution is described using 10 size classes with parallel sections which can have different chemical compositions. Thus in total, the module tracks 20 size sections which cover diameters ranging from 3 nm to 10 μm and are divided into three subranges, each with an optimised selection of processes and compounds. The implementation of SALSA into ECHAM5-HAM includes the main aerosol processes in the atmosphere: emissions, removal, radiative effects, liquid and gas phase sulphate chemistry, and the aerosol microphysics. The aerosol compounds treated in the module are sulphate, organic carbon, sea salt, black carbon, and mineral dust. In its default configuration, ECHAM5-HAM treats aerosol size distribution using the modal method. In this implementation, the aerosol processes were converted to be used in a sectional model framework. The ability of the module to describe the global aerosol properties was evaluated by comparing against (1) measured continental and marine size distributions, (2) observed variability of continental number concentrations, (3) measured sulphate, organic carbon, black carbon and sea-salt mass concentrations, (4) observations of aerosol optical depth (AOD) and other aerosol optical properties from satellites and AERONET network, (5) global aerosol budgets and concentrations from previous model studies, and (6) model results using M7, which is the default aerosol microphysics module in ECHAM5-HAM. The evaluation shows that the global aerosol properties can be reproduced reasonably well using a coarse resolution of 10 sections in size space. The simulated global aerosol budgets are within the range of previous studies. Surface concentrations of sulphate and carbonaceous species have an annual mean within a factor of two of the observations. The simulated sea-salt concentrations reproduce the observations within a factor of two, apart from the Southern Ocean over which the concentrations are within a factor of five. Regionally, AOD is in a relatively good agreement with the observations (within a factor of two). At mid-latitudes the observed AOD is captured well, while at high-latitudes as well as in some polluted and dust regions the modelled AOD is significantly lower than observed. Regarding most of the investigated aerosol properties, the SALSA and the modal aerosol module M7 perform comparably well against observations. However, SALSA reproduces the observed number concentrations and the size distribution of CCN sized particles much more accurately than M7, and is therefore a good choice for aerosol-cloud interaction studies in global models. Our study also shows that when activation type nucleation in the boundary layer is included, the observed concentration of particles under 50 nm in diameter are reproduced much better compared to when only binary nucleation in the free troposphere is assumed.


2005 ◽  
Vol 62 (2) ◽  
pp. 261-285 ◽  
Author(s):  
Vitaly I. Khvorostyanov ◽  
Judith A. Curry

Abstract The new theory of ice nucleation by heterogeneous freezing of deliquescent mixed cloud condensation nuclei (CCN) presented in Part I is incorporated into a parcel model with explicit water and ice bin microphysics to simulate the process of ice nucleation under transient thermodynamic conditions. Simulations are conducted over the temperature range −4° to −60°C, with vertical velocities varying from 1 to 100 cm s−1, for varying initial relative humidities and aerosol characteristics. These simulations show that the same CCN that are responsible for the drop nucleation may initiate crystal nucleation and can be identified as ice nuclei (IN) when crystals form. The simulated nucleation rates and concentrations of nucleated crystals depend on temperature and supersaturation simultaneously, showing good agreement with observations but with noticeable differences when compared with classical temperature-only and supersaturation-only parameterizations. The kinetics of heterogeneous ice nucleation exhibits a negative feedback via water supersaturation, whereby ice nucleation depends on the water supersaturation that is diminished by ice crystal diffusional growth. This feedback is stronger than the corresponding feedback for drop nucleation, and may explain discrepancies between observed ice nuclei concentrations and ice crystal concentrations, the very small fraction of CCN that may serve as IN, and the much smaller crystal concentrations as compared to drop concentrations. The relative importance of heterogeneous versus homogeneous nucleation is examined for a variety of cloud conditions. Based on these calculations, a simple parameterization for ice crystal concentration is suggested for use in cloud models and large-scale models.


2017 ◽  
Vol 14 (2) ◽  
Author(s):  
Kaitlin DuPaul ◽  
Adam Whitten

A synthetic set of aerosol optical depths (AODs) generated from a standard set of aerosol size distributions was analyzed by a parameter based particle swarm optimization (PBPSO) routine in order to test the reproducibility of the results. Junge and lognormal size distributions were consistently reproduced. Gamma and bimodal distributions showed large variability in solutions. values were used to determine the best subset of possible solutions allowing quantification of parameters with uncertainties when using PBPSO. AODs measured by a sun photometer on a clear day (20160413) and a foggy day (20160508) were then processed by the PBPSO program for both bimodal and lognormal distributions. Results showed that in general the foggy day has smaller values indicating that the PBPSO algorithm is better able to match AODs when there is a larger aerosol load in the atmosphere. The bimodal distribution from the clear day best describes the aerosol size distribution since the values are lower. The lognormal distribution best describes the aerosol size distribution on the foggy day (20160508). KEYWORDS: Atmospheric Aerosols; Size Distributions; Junge; Bimodal; Gamma; Lognormal; Particle Swarm Optimization; Inverse Problem; Aerosol Optical Depth


2008 ◽  
Vol 8 (4) ◽  
pp. 15665-15698 ◽  
Author(s):  
D. Barahona ◽  
A. Nenes

Abstract. We present a parameterization of cirrus cloud formation that computes the ice crystal number and size distribution under the presence of homogeneous and heterogeneous freezing. The parameterization is very simple to apply and is derived from the analytical solution of the cloud parcel equations, assuming that the ice nuclei population is monodisperse and chemically homogeneous. In addition to the ice distribution, an analytical expression is provided for the limiting ice nuclei number concentration that suppresses ice formation from homogeneous freezing. The parameterization is evaluated against a detailed numerical parcel model, and reproduces numerical simulations over a wide range of conditions with an average error of 6±33%.


2011 ◽  
Vol 11 (11) ◽  
pp. 29601-29646 ◽  
Author(s):  
D. Barahona

Abstract. This work presents a novel formulation of the ice nucleation spectrum, i.e. the function relating the ice crystal concentration to cloud formation conditions and aerosol properties. The new formulation relies on a statistical view of the ice nucleation process and explicitly accounts for the dependency of the ice crystal concentration on temperature, supersaturation, cooling rate, and particle size, and, in the case of heterogeneous ice nucleation, on the distributions of particle area and surface composition. The new formulation is used to generate ice nucleation parameterizations for the homogeneous freezing of cloud droplets and the heterogeneous deposition ice nucleation on dust and soot ice nuclei. For homogeneous freezing, it was found that by increasing the dispersion in the droplet volume distribution the fraction of supercooled droplets in the population increases. For heterogeneous ice nucleation it was found that ice nucleation on efficient ice nuclei (IN) shows features consistent with the singular hypothesis (characterized by a lack of temporal dependency of the ice nucleation spectrum) whereas less efficient IN tend to display stochastic behavior. Analysis of empirical nucleation spectra suggested that inferring the aerosol heterogeneous ice nucleation properties from measurements of the onset supersaturation and temperature may carry significant error as the variability in ice nucleation properties within the aerosol population is not accounted for. This work provides a simple and rigorous ice nucleation framework were theoretical predictions, laboratory measurements and field campaign data can be reconciled, and that is suitable for application in atmospheric modeling studies.


2012 ◽  
Vol 12 (24) ◽  
pp. 12061-12079 ◽  
Author(s):  
X. Liu ◽  
X. Shi ◽  
K. Zhang ◽  
E. J. Jensen ◽  
A. Gettelman ◽  
...  

Abstract. In this study the effect of dust aerosol on upper tropospheric cirrus clouds through heterogeneous ice nucleation is investigated in the Community Atmospheric Model version 5 (CAM5) with two ice nucleation parameterizations. Both parameterizations consider homogeneous and heterogeneous nucleation and the competition between the two mechanisms in cirrus clouds, but differ significantly in the number concentration of heterogeneous ice nuclei (IN) from dust. Heterogeneous nucleation on dust aerosol reduces the occurrence frequency of homogeneous nucleation and thus the ice crystal number concentration in the Northern Hemisphere (NH) cirrus clouds compared to simulations with pure homogeneous nucleation. Global and annual mean shortwave and longwave cloud forcing are reduced by up to 2.0 ± 0.1 W m−2 (1σ uncertainty) and 2.4 ± 0.1 W m−2, respectively due to the presence of dust IN, with the net cloud forcing change of −0.40 ± 0.20 W m−2. Comparison of model simulations with in situ aircraft data obtained in NH mid-latitudes suggests that homogeneous ice nucleation may play an important role in the ice nucleation at these regions with temperatures of 205–230 K. However, simulations overestimate observed ice crystal number concentrations in the tropical tropopause regions with temperatures of 190–205 K, and overestimate the frequency of occurrence of high ice crystal number concentration (> 200 L−1) and underestimate the frequency of low ice crystal number concentration (< 30 L−1) at NH mid-latitudes. These results highlight the importance of quantifying the number concentrations and properties of heterogeneous IN (including dust aerosol) in the upper troposphere from the global perspective.


2009 ◽  
Vol 9 (3) ◽  
pp. 10957-11004 ◽  
Author(s):  
D. Barahona ◽  
A. Nenes

Abstract. This study presents a comprehensive ice cloud formation parameterization that computes the ice crystal number, size distribution, and maximum supersaturation from precursor aerosol and ice nuclei with any size distribution and chemical composition. The parameterization provides an analytical solution of the cloud parcel model equations and accounts for the competition effects between homogeneous and heterogeneous freezing, and, between heterogeneous freezing in different modes. The diversity of heterogeneous nuclei is described through a nucleation spectrum function which is allowed to follow any form (i.e., derived from classical nucleation theory or from empirical observations). The parameterization reproduced the predictions of a detailed numerical parcel model over a wide range of conditions, and several expressions for the nucleation spectrum. The average error in ice crystal number concentration was −2.0±8.5% for conditions of pure heterogeneous freezing, and, 4.7±21% when both homogeneous and heterogeneous freezing were active. Apart from its rigor, excellent performance and versatility, the formulation is extremely fast and free from requirements of numerical integration.


2009 ◽  
Vol 9 (5) ◽  
pp. 20631-20675 ◽  
Author(s):  
E. J. Jensen ◽  
L. Pfister ◽  
T.-P. Bui ◽  
P. Lawson ◽  
D. Baumgardner

Abstract. In past modeling studies, it has generally been assumed that the predominant mechanism for nucleation of ice in the uppermost troposphere is homogeneous freezing of aqueous aerosols. However, recent in situ and remote-sensing measurements of the properties of cirrus clouds at very low temperatures in the tropical tropopause layer (TTL) are broadly inconsistent with theoretial predictions based on the homogeneous freezing assumption. The nearly ubiquitous occurence of gravity waves in the TTL makes the predictions from homogeneous nucleation theory particularly difficult to reconcile with measurements. These measured properties include ice number concentrations, which are much lower than theory predicts; ice crystal size distributions, which are much broader than theory predicts; and cloud extinctions, which are much lower than theory predicts. Although other explanations are possible, one way to limit ice concentrations is to have on the order of 50 L−1 effective ice nuclei (IN) that could nucleate ice at relatively low supersaturations. We suggest that ammonium sulfate particles, which would be dry much of the time in the cold TTL, are a potential IN candidate for TTL cirrus. Possible implications of the observed cloud microphysical properties for ice sedimentation, dehydration, and cloud persistence are also discussed.


2014 ◽  
Vol 14 (11) ◽  
pp. 16493-16528 ◽  
Author(s):  
N. Hiranuma ◽  
M. Paukert ◽  
I. Steinke ◽  
K. Zhang ◽  
G. Kulkarni ◽  
...  

Abstract. A new heterogeneous ice nucleation parameterization that covers a wide temperature range (−36 to −78 °C) is presented. Developing and testing such an ice nucleation parameterization, which is constrained through identical experimental conditions, is critical in order to accurately simulate the ice nucleation processes in cirrus clouds. The surface-scaled ice nucleation efficiencies of hematite particles, inferred by ns, were derived from AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber measurements under water subsaturated conditions that were realized by continuously changing temperature (T) and relative humidity with respect to ice (RHice) in the chamber. Our measurements showed several different pathways to nucleate ice depending on T and RHice conditions. For instance, almost T-independent freezing was observed at −60 °C < T < −50 °C, where RHice explicitly controlled ice nucleation efficiency, while both T and RHice played roles in other two T regimes: −78 °C < T < −60 °C and −50 °C < T < −36 °C. More specifically, observations at T colder than −60 °C revealed that higher RHice was necessary to maintain constant ns, whereas T may have played a significant role in ice nucleation at T warmer than −50 °C. We implemented new ns parameterizations into two cloud models to investigate its sensitivity and compare with the existing ice nucleation schemes towards simulating cirrus cloud properties. Our results show that the new AIDA-based parameterizations lead to an order of magnitude higher ice crystal concentrations and inhibition of homogeneous nucleation in colder temperature regions. Our cloud simulation results suggest that atmospheric dust particles that form ice nuclei at lower temperatures, below −36 °C, can potentially have stronger influence on cloud properties such as cloud longevity and initiation when compared to previous parameterizations.


2009 ◽  
Vol 9 (2) ◽  
pp. 369-381 ◽  
Author(s):  
D. Barahona ◽  
A. Nenes

Abstract. We present a parameterization of cirrus cloud formation that computes the ice crystal number and size distribution under the presence of homogeneous and heterogeneous freezing. The parameterization is very simple to apply and is derived from the analytical solution of the cloud parcel equations, assuming that the ice nuclei population is monodisperse and chemically homogeneous. In addition to the ice distribution, an analytical expression is provided for the limiting ice nuclei number concentration that suppresses ice formation from homogeneous freezing. The parameterization is evaluated against a detailed numerical parcel model, and reproduces numerical simulations over a wide range of conditions with an average error of 6±33%. The parameterization also compares favorably against other formulations that require some form of numerical integration.


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