Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “Cloud parameterizations”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 181 records · Page 10

Application of the NASA A-Train to Evaluate Clouds Simulated by the Weather Research and Forecast Model

The CloudSat Mission, part of the NASA A-Train, is providing the first global survey of cloud profiles and cloud physical properties, observing seasonal and geographical variations that are pertinent to evaluating the way clouds are parameterized in weather and climate forecast models. CloudSat measures the vertical structure of clouds and precipitation from space through the Cloud Profiling Radar (CPR), a 94 GHz nadir-looking radar measuring the power backscattered by clouds as a function of distance from the radar. One of the goals of the CloudSat mission is to evaluate the representation of clouds in forecast models, thereby contributing to improved predictions of weather, climate and the cloud-climate feedback problem. This paper highlights potential limitations in cloud microphysical schemes currently employed in the Weather Research and Forecast (WRF) modeling system. The horizontal and vertical structure of explicitly simulated cloud fields produced by the WRF model at 4-km resolution are being evaluated using CloudSat observations in concert with products derived from MODIS and AIRS. A radiative transfer model is used to produce simulated profiles of radar reflectivity given WRF input profiles of hydrometeor mixing ratios and ambient atmospheric conditions. The preliminary results presented in the paper will compare simulated and observed reflectivity fields corresponding to horizontal and vertical cloud structures associated with midlatitude cyclone events.

Molthan, Andrew L.↗

The Ice Particle and Aggregate Simulator (IPAS). Part II: Analysis of a Database of Theoretical Aggregates for Microphysical Parameterization

Abstract Bulk ice-microphysical models parameterize the dynamic evolution of ice particles from advection, collection, and sedimentation through a cloud layer to the surface. Frozen hydrometeors can grow to acquire a multitude of shapes and sizes, which influence the distribution of mass within cloud systems. Aggregates, defined herein as the collection of ice particles, have a variety of formations based on initial ice particle size, shape, falling orientation, and the number of particles that collect. This work focuses on using the Ice Particle and Aggregate Simulator (IPAS) as a statistical tool to repetitively collect ice crystals of identical properties to derive bulk aggregate characteristics. A database of 9 744 000 aggregates is generated with resulting properties analyzed. After 150 single ice crystals (monomers) collect, the most extreme aggregate aspect ratio calculations asymptote toward and ϕ ca ≈ 0.50 for aggregates composed of quasi-horizontally oriented and randomly oriented monomers, respectively. The results presented are largely consistent with both a previous theoretical study and estimates derived from ground-based observations from two different geographic locations. Particle falling orientation highly influences newly formed aggregate aspect ratios from the collection of particles with extreme aspect ratios; quasi-horizontally oriented particles can produce aggregate aspect ratios an order of magnitude more extreme than randomly oriented particles but can also produce near-spherical aggregates as the number of monomers comprising the aggregate reach approximately 100. Finally, a majority of collections result in aggregates that are closer to prolate than oblate spheroids.

54 ENVIRONMENTAL SCIENCES↗

Incorporation of multiple cloud layers for ultraviolet radiation modeling studies

Cloud data sets compiled from surface observations were used to develop an algorithm for incorporating multiple cloud layers into a multiple-scattering radiative transfer model. Aerosol extinction and ozone data sets were also incorporated to estimate the seasonally averaged ultraviolet (UV) flux reaching the surface of the Earth in the Detroit, Michigan, region for the years 1979-1991, corresponding to Total Ozone Mapping Spectrometer (TOMS) version 6 ozone observations. The calculated UV spectrum was convolved with an erythema action spectrum to estimate the effective biological exposure for erythema. Calculations show that decreasing the total column density of ozone by 1% leads to an increase in erythemal exposure by approximately 1.1-1.3%, in good agreement with previous studies. A comparison of the UV radiation budget at the surface between a single cloud layer method and a multiple cloud layer method presented here is discussed, along with limitations of each technique. With improved parameterization of cloud properties, and as knowledge of biological effects of UV exposure increase, inclusion of multiple cloud layers may be important in accurately determining the biologically effective UV budget at the surface of the Earth.

Charache, Darryl H.↗

Implementation of Cloud Retrievals for Tropospheric Emission Spectrometer (TES) Atmospheric Retrievals: Part 1. Description and Characterization of Errors on Trace Gas Retrievals

We develop an approach to estimate and characterize trace gas retrievals in the presence of clouds in high spectral measurements of upwelling radiance in the infrared spectral region (650-2260/cm). The radiance contribution of clouds is parameterized in terms of a set of frequency-dependent nonscattering optical depths and a cloud height. These cloud parameters are retrieved jointly with surface temperature, emissivity, atmospheric temperature, and trace gases such as ozone from spectral data. We demonstrate the application of this approach using data from the Tropospheric Emission Spectrometer (TES) and test data simulated with a scattering radiative transfer model. We show the value of this approach in that it results in accurate estimates of errors for trace gas retrievals, and the retrieved values improve over the initial guess for a wide range of cloud conditions. Comparisons are made between TES retrievals of ozone, temperature, and water to model fields from the Global Modeling and Assimilation Office (GMAO), temperature retrievals from the Atmospheric Infrared Sounder (AIRS), tropospheric ozone columns from the Goddard Earth Observing System (GEOS) GEOS-Chem, and ozone retrievals from the Total Ozone Mapping Spectrometer (TOMS). In each of these cases, this cloud retrieval approach does not introduce observable biases into TES retrievals.

aerosols↗

IR spectral characteristics of cirrus clouds

The recent focus of parameterization of the radiative properties of clouds has been to include the microphysical properties of the cloud. A variety of parameterization have been developed for both the shortwave and the longwave. In parameterizing the longwave properties of clouds, it is useful to consider the two stream solution of the radiative transfer equation appropriate for a thermal source. These radiative transfer equations are considered.

Ackerman, Steven A.↗

A Study of the Relationship Between Anthropogenic Sulfate and Cloud Drop Nucleation

The characteristics of the cloud drop size distribution near cloud base are initially determined by the aerosol particles that serve as CCN and by the local updraft velocity. Chemical reactions of the emitted gaseous sulfur compounds due to human activities will alter, through gas-to-particle conversion, the aerosol size distribution, total number, and its chemical composition. Recently, Boucher and Rodhe and Jones et.al have each developed parameterizations relating cloud drop concentration to sulfate mass or aerosol number concentration, respectively, and used them to develop estimates of the indirect forcing by anthropogenic sulfate aerosols. THese parameterizations made use of measure relationships in continental and maritime clouds. However, these relationships are inherently noisy, yielding more than a factor of 2 variation in cloud drop concentration for a given aerosol number (or for a given sulfate mass) concentration. The large spatial and temporal variabilities in the concentration, chemical characteristics, and size distribution of aerosols have made it difficult to develop such a parameterization from data. In this paper, our focus is to develop a means for relating the predicted anthropogenic sulfate mass to cloud drop number concentration over the range of expected conditions associated with continental and marine aerosol. We start with an assumed pre-existing particle size distribution and develop an approximation of the altered distribution after addition of anthropogenic sulfate. We thereby develop a conservative estimate of the possible change in cloud drop number concentration due to anthropogenic sulfate.

Chuang, Catherine C.↗

Modeling of Sub-Grid Heterogeneity and its Impact on GCM Global Radiation Balance

The spatial and temporal variability of high, low, and mid-level clouds is obtained from ISCCP D1 data. Monthly mean global maps of the observed cloud variability are used to re-scale GCM prognostic cloud optical depths and radiative parameters via the Monte Carlo cloud heterogeneity parameterization that utilizes the existing plane-parallel GCM radiative transfer model to compute radiative fluxes for inhomogeneous cloud distributions. The GCM radiative fluxes at TOA and the ground surface are then compared to ERBE and GEBA results. These comparisons show that including sub-grid cloud variability in the GCM radiative model improves agreement between the GCM radiative energy budget components and observations,

Lacis, Andrew↗

The Role of Deep Convection and Large-scale Circulation in Driving Model Spread in Low Cloud Feedback and Equilibrium Climate Sensitivity

This project aims to advance the understanding of the processes that drive the large uncertainties in climate change projections, use observations to constrain model physics and reduce the inter-model spread in equilibrium climate sensitivity (ECS). There are three major goals: 1) Characterize the representation of the physical pathways that link deep convection, large-scale circulation and low cloud feedback in CMIP6 model simulations and determine the relative contribution of each pathway to the CMIP6 model spread in low cloud feedback and ECS; 2) Use process-oriented diagnostics and multiple observations to evaluate CMIP6 model performance in capturing the observed cloud-circulation relation and deep convection characteristics including convective transition statistics and the bulk properties of mesoscale convective systems (MCSs). Error decomposition in CMIP6 models will be performed. 3) Conduct E3SM short-range hindcasts following the DOE Cloud-Associated Parameterizations Testbed (CAPT) protocol to pinpoint specific model parameters/processes that are crucial to the representation of deep convection, circulation, clouds and the pathways that connect them. We will modify convective parameters in E3SM and analyze the perturbed physics experiments (PPEs) to isolate model parameters that are critical to the uncertainty of ECS.

54 ENVIRONMENTAL SCIENCES↗

Implementation and Evaluation of Physics-Driven Dynamic Entrainment-Mixing Parameterization in a Climate Model and Its Impact on Low-Cloud Simulation

The turbulent entrainment-mixing process in the Community Earth System Model version 1.2 (CESM1.2) is assumed to follow the extremely inhomogeneous entrainment-mixing. However, different entrainment-mixing scenarios can occur in real clouds. To address this deficiency, a unifying parameterization that represents different entrainment-mixing processes is implemented and evaluated in CESM1.2. The results indicate that the homogeneous mixing degree values simulated by the new parameterization in CESM1.2 are predominantly greater than 50%, suggesting a tendency toward homogeneous mixing. Compared to the extremely inhomogeneous mixing mechanism, the new parameterization increases the cloud droplet number concentration (Nc). More importantly, the new parameterization improves low-cloud fraction (CLDLOW) simulation in Northwest Pacific (NWP) and Southeast Pacific (SEP) regions, with relative improvements of 2.95% and 4.17%, respectively. Furthermore, the improvements reach up to 44.6% and 16.2% in the NWP and SEP regions, respectively, when considering the relationship between N c and CLDLOW. Further analysis reveals that the new parameterization enhances cloud optical depth, longwave radiative cooling effect, net condensation rate, cloud water mixing ratio, lower-troposphere stability, and CLDLOW by increasing N c . Additionally, these results underscore the importance of improving entrainment-mixing parameterization in climate models.

54 ENVIRONMENTAL SCIENCES↗

Cloud optical parameters as derived from the multispectral cloud radiometer

Simultaneous measurements of the liquid water content and particle size have assumed an important role in cloud physics as they help elucidate the mechanism of cloud particle formation and the mechanism of air mass-mixing in stratus clouds. Such measurements can reveal the modification of cloud air masses by anthropogenic aerosol particles (Coakley et al. 1987, Durkee 1989). Studies of the climatic impact of these modification processes on cloud microphysics seems to be urgent for understanding mechanisms of climate change. General Circulation Model (GCM) simulations can be improved by introducing a parameterization of cloud optical properties in terms of integrated liquid water content (liquid water path) and particle size (Slingo 1989). Motivated by the above mentioned circumstances, remote sensing techniques were developed for simultaneously retrieving the cloud optical thickness and effective particle radius, from which the liquid water path can be inferred. Statistical features of the cloud optical thickness (or liquid water path) and effective particle size for marine stratocumulus clouds are presented. These results were obtained during 4 days (7, 10, 13, and 16 July 1987) of observations with the Multispectral Cloud Radiometer (ER-2) and the Thematic Mapper (LANDSAT-5) during the First ISCCP Regional Experiment (FIRE).

Nakajima, Teruyuki↗

Physical retrieval of precipitation water contents from Special Sensor Microwave/Imager (SSM/I) data. Part 2: Retrieval method and applications (report version)

A physical retrieval method for estimating precipitating water distributions and other geophysical parameters based upon measurements from the DMSP-F8 SSM/I is developed. Three unique features of the retrieval method are (1) sensor antenna patterns are explicitly included to accommodate varying channel resolution; (2) precipitation-brightness temperature relationships are quantified using the cloud ensemble/radiative parameterization; and (3) spatial constraints are imposed for certain background parameters, such as humidity, which vary more slowly in the horizontal than the cloud and precipitation water contents. The general framework of the method will facilitate the incorporation of measurements from the SSMJT, SSM/T-2 and geostationary infrared measurements, as well as information from conventional sources (e.g., radiosondes) or numerical forecast model fields.

Olson, William S.↗

Parameterization of radiative flux profiles within layer clouds

This paper presents simple formulations for the vertical structure of solar and infrared radiative fluxes within a layer cloud overlying a partially reflective surface. The parameterized profile shapes are analytic, with governing parameters derived from bulk radiative properties and more physically based radiative transfer models. The bulk cloud, subcloud layer, and surface radiative properties are assumed to be known. The parameterizations are based on exponential functions of height, with decay scales related to cloud liquid water content. Although the results presented here are based on very simple assumptions about the cloud structure in the vertical, the method used is applicable to more general cases as well as to various other analytic and/or numerical radiative transfer calculations.

Hanson, Howard P.↗

Understanding Changes in Cloud Simulations from E3SM Version 1 to Version 2

This study documents clouds simulated by the Energy Exascale Earth System Model (E3SM) version 2 (E3SMv2) and attempts to understand what causes the model behavior change in clouds relative to E3SMv1. This is done by analyzing the last 30-year (1985–2014) data from the 165-year historical simulations using E3SMv1 and v2 and four sensitivity tests to isolate the impact of changes in model parameter choices in its turbulence, shallow convection, and cloud macrophysics parameterization (CLUBB), microphysical parameterization (MG2), and deep convection scheme (ZM), as well as model physics changes in convective triggering. It is shown that E3SMv2 significantly improves the simulation of subtropical coastal stratocumulus clouds (Sc) and clouds with optical depth larger than 3.6 over the stratocumulus to cumulus transition regimes, where Shortwave Cloud Radiative Effect (SWCRE) is also improved, and the Southern Ocean (SO) while seeing an overall slight degradation in low clouds over other tropical and subtropical oceans. The better performance in E3SMv1 over those regions is partially due to error compensation between its simulated optically thin and intermediate low clouds for which E3SMv2 actually improves simulation of optically intermediate low clouds. Sensitivity tests indicate that the changes in low clouds are primarily due to the tuning made in CLUBB. The impact of the ZM tuning is mainly on optically intermediate and thick high clouds, contributing to improved SWCRE and Longwave Cloud Radiative Effect (LWCRE). The impact of the MG2 tuning and the new convective trigger is primarily on the high latitudes and the Southern Ocean (SO). They have a relatively smaller impact on clouds than do the CLUBB and ZM tunings. This study offers additional insights about clouds simulated in E3SMv2 by utilizing multiple data sets and the COSP diagnostic tool as well as through sensitivity tests. The improved understanding will benefit the future E3SM developments.

54 ENVIRONMENTAL SCIENCES↗

Impact of the Ozone Monitoring Instrument Row Anomaly on the Long-Term Record of Aerosol Products

Since about three years after the launch the Ozone Monitoring Instrument (OMI) on the EOS-Aura satellite, the sensor's viewing capability has been affected by what is believed to be an internal obstruction that has reduced OMI's spatial coverage. It currently affects about half of the instrument's 60 viewing positions. In this work we carry out an analysis to assess the effect of the reduced spatial coverage on the monthly average values of retrieved aerosol optical depth (AOD), single scattering albedo (SSA) and the UV Aerosol Index (UVAI) using the 2005-2007 three-year period prior to the onset of the row anomaly. Regional monthly average values calculated using viewing positions 1 through 30 were compared to similarly obtained values using positions 31 through 60, with the expectation of finding close agreement between the two calculations. As expected, mean monthly values of AOD and SSA obtained with these two scattering-angle dependent subsets of OMI observations agreed over regions where carbonaceous or sulphate aerosol particles are the predominant aerosol type. However, over arid regions, where desert dust is the main aerosol type, significant differences between the two sets of calculated regional mean values of AOD were observed. As it turned out, the difference in retrieved desert dust AOD between the scattering-angle dependent observation subsets was due to the incorrect representation of desert dust scattering phase function. A sensitivity analysis using radiative transfer calculations demonstrated that the source of the observed AOD bias was the spherical shape assumption of desert dust particles. A similar analysis in terms of UVAI yielded large differences in the monthly mean values for the two sets of calculations over cloudy regions. On the contrary, in arid regions with minimum cloud presence, the resulting UVAI monthly average values for the two sets of observations were in very close agreement. The discrepancy under cloudy conditions was found to be caused by the parameterization of clouds as opaque Lambertian reflectors. When properly accounting for cloud scattering effects using Mie theory, the observed UVAI angular bias was significantly reduced. The analysis discussed here has uncovered important algorithmic deficiencies associated with the model representation of the angular dependence of scattering effects of desert dust aerosols and cloud droplets. The resulting improvements in the handling of desert dust and cloud scattering have been incorporated in an improved version of the OMAERUV algorithm.

Atmospheric Chemistry↗

Large Eddy Simulation of Cirrus Clouds

The Regional Atmospheric Modeling System (RAMS) with mesoscale interactive nested-grids and a Large-Eddy Simulation (LES) version of RAMS, coupled to two-moment microphysics and a new two-stream radiative code were used to investigate the dynamic, microphysical, and radiative aspects of the November 26, 1991 cirrus event. Wu (1998) describes the results of that research in full detail and is enclosed as Appendix 1. The mesoscale nested grid simulation successfully reproduced the large scale circulation as compared to the Mesoscale Analysis and Prediction System's (MAPS) analyses and other observations. Three cloud bands which match nicely to the three cloud lines identified in an observational study (Mace et al., 1995) are predicted on Grid #2 of the nested grids, even though the mesoscale simulation predicts a larger west-east cloud width than what was observed. Large-eddy simulations (LES) were performed to study the dynamical, microphysical, and radiative processes in the 26 November 1991 FIRE 11 cirrus event. The LES model is based on the RAMS version 3b developed at Colorado State University. It includes a new radiation scheme developed by Harrington (1997) and a new subgrid scale model developed by Kosovic (1996). The LES model simulated a single cloud layer for Case 1 and a two-layer cloud structure for Case 2. The simulations demonstrated that latent heat release can play a significant role in the formation and development of cirrus clouds. For the thin cirrus in Case 1, the latent heat release was insufficient for the cirrus clouds to become positively buoyant. However, in some special cases such as Case 2, positively buoyant cells can be embedded within the cirrus layers. These cells were so active that the rising updraft induced its own pressure perturbations that affected the cloud evolution. Vertical profiles of the total radiative and latent heating rates indicated that for well developed, deep, and active cirrus clouds, radiative cooling and latent heating could be comparable in magnitude in the cloudy layer. This implies that latent heating cannot be neglected in the construction of a cirrus cloud model. The probability density function (PDF) of w was analyzed to assist in the parameterization of cloud-scale velocities in large-scale models. For the more radiatively-driven, thin cirrus case, the PDFs are approximately Gaussian. However, in the interior of the deep, convectively unstable case, the PDFs of w are multi-modal and very broad, indicating that parameterizing cloud-scale motions for such clouds can be very challenging. The results of this research are described in detail in a paper submitted to the Journal of Atmospheric Science (Wu and Cotton, 1999), which is enclosed as Appendix 2. Using soundings extracted from a mesoscale simulation of the November 26, 1991 cirrus event, the radiative effects on vapor deposition/sublimation of ice crystals was studied using a two-dimensional cloud-resolving model (CRM) version of RAMS, coupled to an explicit bin-resolving microphysics. The CRM simulations of the November 26, 1991 cirrus event demonstrate that the radiative impact on the diffusional growth (or sublimation) of ice crystals is significant. In this case, the ice particles experienced radiative warming. Model results show that radiative feedbacks in the diffusional growth of ice particles can be very complex. Radiative warming of an ice particle will restrict the particle's diffusional growth. In the case of radiative warming, ice particles larger than a certain size will experience so much radiative warming that surface ice saturation vapor pressures become large enough to cause sublimation of the larger crystals, while smaller crystals are growing by vapor deposition. However, ice mass production can be enhanced in the case of radiative cooling of an ice particle. For the November 26, 1991 cirrus event, radiative feedback results in significant reduction in the total ice mass, especially in the production of large ice crystals, and consequently, both radiative and dynamic properties of the cirrus cloud are significantly affected. A complete description of this research has been submitted as a paper to the Journal of Atmospheric Science (Wu et al., 1999), and included as Appendix 3.

Wu, Ting↗

Overview and Statistical Analysis of Boundary Layer Clouds and Precipitation Over the Western North Atlantic Ocean

Due to their fast evolution and large natural variability in macro- and microphysical properties, the accurate representation of boundary layer clouds in current climate models remains a challenge. One of the regions with large intermodel spread in the Coupled Model Intercomparison Project Phase 6 ensemble is the western North Atlantic Ocean. Here, statistically representative in situ measurements can help to develop and constrain the parameterization of clouds in global models. To this end, we performed comprehensive measurements of boundary layer clouds, aerosol, trace gases, and radiation in the western North Atlantic Ocean during the NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) mission. In total, 174 research flights with 574 flight hours for cloud and precipitation measurements were performed with the HU-25 Falcon during three winter (February–March 2020, January–April 2021, and November 2021–March 2022) and three summer seasons (August–September 2020, May–June 2021, and May–June 2022). Here we present a statistical evaluation of 16 140 individual cloud events probed by the fast cloud droplet probe and the two-dimensional stereo cloud probe during 155 research flights in a representative and repetitive flight strategy allowing for robust statistical data analyses. We show that the vertical profiles of distributions of the liquid water content and the cloud droplet effective diameter (ED) increase with altitude in the marine boundary layer. Due to higher updraft speeds, higher cloud droplet number concentrations (N liquid ) were measured in winter compared to summer despite lower cloud condensation nucleus abundance. Flight cloud cover derived from statistical analysis of in situ data is reduced in summer and shows large variability. This seasonal contrast in cloud coverage is consistent with a dominance of a synoptic pattern in winter that favors conditions for the formation of stratiform clouds at the western edge of cyclones (post-cyclonic). In contrast, a dominant summer anticyclone is concomitant with the occurrence of shallow cumulus clouds and lower cloud coverage. The evaluation of boundary layer clouds and precipitation in the N liquid ED phase space sheds light on liquid, mixed-phase, and ice cloud properties and helps to categorize the cloud data. Ice and liquid precipitation, often masked in cloud statistics by a high abundance of liquid clouds, is often observed throughout the cloud. The ACTIVATE in situ cloud measurements provide a wealth of cloud information useful for assessing airborne and satellite remote-sensing products, for global climate and weather model evaluations, and for dedicated process studies that address precipitation and aerosol–cloud interactions.

Aerosol↗

Limitations of Separate Cloud and Rain Categories in Parameterizing Collision-Coalescence for Bulk Microphysics Schemes

Warm rain collision-coalescence has been persistently difficult to parameterize in bulk microphysics schemes. We use a flexible bulk microphysics scheme with bin scheme process parameterizations, called AMP, to investigate reasons for the difficulty. AMP is configured in a variety of ways to mimic bulk schemes and is compared to simulations with the bin scheme upon which AMP is built. We find that an important limitation in traditional bulk schemes is the use of separate cloud and rain categories. When the drop size distribution is instead represented by a continuous distribution, the simulation of cloud-to-rain conversion is substantially improved. We also find large sensitivity to the threshold size to distinguish cloud and rain in traditional schemes; substantial improvement is found by decreasing the threshold from 40 to 25 μm. Neither the use of an assumed functional form for the size distribution nor the choice of predicted distribution moments has a large impact on the ability of AMP to simulate rain production. When predicting four total moments of the liquid drop size distribution, either with a traditional two-category, two-moment scheme with a reduced size threshold, or a four-moment single-category scheme, errors in the evolution of mass and the cloud size distribution are similar, but the single-category scheme has a substantially better representation of the rain size distribution. Optimal moment combinations for the single-category approach are investigated and appear to be linked more to the information content they provide for constraining the size distributions than to their correlation with collision-coalescence rates.

autoconversion↗

Thermodynamic Derivation of the Activation Energy for Ice Nucleation

Cirrus clouds play a key role in the radiative and hydrological balance of the upper troposphere. Their correct representation in atmospheric models requires an understanding of the microscopic processes leading to ice nucleation. A key parameter in the theoretical description of ice nucleation is the activation energy, which controls the flux of water molecules from the bulk of the liquid to the solid during the early stages of ice formation. In most studies it is estimated by direct association with the bulk properties of water, typically viscosity and self-diffusivity. As the environment in the ice-liquid interface may differ from that of the bulk, this approach may introduce bias in calculated nucleation rates. In this work a theoretical model is proposed to describe the transfer of water molecules across the ice-liquid interface. Within this framework the activation energy naturally emerges from the combination of the energy required to break hydrogen bonds in the liquid, i.e., the bulk diffusion process, and the work dissipated from the molecular rearrangement of water molecules within the ice-liquid interface. The new expression is introduced into a generalized form of classical nucleation theory. Even though no nucleation rate measurements are used to fit any of the parameters of the theory the predicted nucleation rate is in good agreement with experimental results, even at temperature as low as 190 K, where it tends to be underestimated by most models. It is shown that the activation energy has a strong dependency on temperature and a weak dependency on water activity. Such dependencies are masked by thermodynamic effects at temperatures typical of homogeneous freezing of cloud droplets; however, they may affect the formation of ice in haze aerosol particles. The new model provides an independent estimation of the activation energy and the homogeneous ice nucleation rate, and it may help to improve the interpretation of experimental results and the development of parameterizations for cloud formation.

Cirrus clouds↗