scholarly journals Liquid-like layers on ice in the environment: bridging the quasi-liquid and brine layer paradigms

2011 ◽  
Vol 11 (3) ◽  
pp. 8145-8172 ◽  
Author(s):  
M. H. Kuo ◽  
S. G. Moussa ◽  
V. F. McNeill

Abstract. Liquid-like layers on ice significantly influence atmospheric chemistry in polar regions. In the absence of impurities a nanoscale region of surface disorder known as the "quasi-liquid layer" (QLL) may exist below the bulk melting point (down to ~−30 °C). Surface and bulk impurities are known to modulate the QLL thickness. In aqueous systems containing ionic solutes, a liquid brine layer (BL) may form upon freezing due to the exclusion of impurities from the ice crystal lattice coupled with freezing point depression in the concentrated surface layer. Brine layers are conceptually distinct from the QLL, which can exist in the absence of impurities. We have developed a unified model for liquid-like layers in environmental ice systems that is valid over a wide range of temperatures and solute concentrations, spanning the QLL and BL regimes. The model consists of two coupled modules describing the thickness of the BL and the QLL. The BL module is derived from fundamental equlibrium thermodynamics, whereas the QLL formulation is derived semi-empirically based on statistical mechanical principles and previously published QLL thickness data. The resulting unified model has been tested against experimental data from literature and applied to several environmentally important systems, such as HCl(g)-ice, HNO3(g)-ice, and frozen sea ice. This model can be used to improve the representation of air-ice chemical interactions in polar atmospheric chemistry models.

2011 ◽  
Vol 11 (18) ◽  
pp. 9971-9982 ◽  
Author(s):  
M. H. Kuo ◽  
S. G. Moussa ◽  
V. F. McNeill

Abstract. Interfacial layers on ice significantly influence air-ice chemical interactions. In solute-containing aqueous systems, a liquid brine may form upon freezing due to the exclusion of impurities from the ice crystal lattice coupled with freezing point depression in the concentrated brine. The brine may be segregated to the air-ice interface where it creates a surface layer, in micropockets, or at grain boundaries or triple junctions. We present a model for brines and their associated liquid layers in environmental ice systems that is valid over a wide range of temperatures and solute concentrations. The model is derived from fundamental equlibrium thermodynamics and takes into account nonideal solution behavior in the brine, partitioning of the solute into the ice matrix, and equilibration between the brine and the gas phase for volatile solutes. We find that these phenomena are important to consider when modeling brines in environmental ices, especially at low temperatures. We demonstrate its application for environmentally important volatile and nonvolatile solutes including NaCl, HCl, and HNO3. The model is compared to existing models and experimental data from literature where available. We also identify environmentally relevant regimes where brine is not predicted to exist, but the QLL may significantly impact air-ice chemical interactions. This model can be used to improve the representation of air-ice chemical interactions in polar atmospheric chemistry models.


Atmosphere ◽  
2021 ◽  
Vol 12 (6) ◽  
pp. 680
Author(s):  
Chris D. Boone ◽  
Johnathan Steffen ◽  
Jeff Crouse ◽  
Peter F. Bernath

Line-of-sight wind profiles are derived from Doppler shifts in infrared solar occultation measurements from the Atmospheric Chemistry Experiment Fourier transform spectrometers (ACE-FTS), the primary instrument on SCISAT, a satellite-based mission for monitoring the Earth’s atmosphere. Comparisons suggest a possible eastward bias from 20 m/s to 30 m/s in ACE-FTS results above 80 km relative to some datasets but no persistent bias relative to other datasets. For instruments operating in a limb geometry, looking through a wide range of altitudes, smearing of the Doppler effect along the line of sight can impact the measured signal, particularly for saturated absorption lines. Implications of Doppler effect smearing are investigated for forward model calculations and volume mixing ratio retrievals. Effects are generally small enough to be safely ignored, except for molecules having a large overhang in their volume mixing ratio profile, such as carbon monoxide.


2013 ◽  
Vol 6 (1) ◽  
pp. 453-494 ◽  
Author(s):  
D. S. Moreira ◽  
S. R. Freitas ◽  
J. P. Bonatti ◽  
L. M. Mercado ◽  
N. M. É. Rosário ◽  
...  

Abstract. This article presents the development of a new numerical system denominated JULES-CCATT-BRAMS, which resulted from the coupling of the JULES surface model to the CCATT-BRAMS atmospheric chemistry model. The performance of this system in relation to several meteorological variables (wind speed at 10 m, air temperature at 2 m, dew point temperature at 2 m, pressure reduced to mean sea level and 6 h accumulated precipitation) and the CO2 concentration above an extensive area of South America is also presented, focusing on the Amazon basin. The evaluations were conducted for two periods, the wet (March) and dry (September) seasons of 2010. The statistics used to perform the evaluation included bias (BIAS) and root mean squared error (RMSE). The errors were calculated in relation to observations at conventional stations in airports and automatic stations. In addition, CO2 concentrations in the first model level were compared with meteorological tower measurements and vertical CO2 profiles were compared with aircraft data. The results of this study show that the JULES model coupled to CCATT-BRAMS provided a significant gain in performance in the evaluated atmospheric fields relative to those simulated by the LEAF (version 3) surface model originally utilized by CCATT-BRAMS. Simulations of CO2 concentrations in Amazonia and a comparison with observations are also discussed and show that the system presents a gain in performance relative to previous studies. Finally, we discuss a wide range of numerical studies integrating coupled atmospheric, land surface and chemistry processes that could be produced with the system described here. Therefore, this work presents to the scientific community a free tool, with good performance in relation to the observed data and re-analyses, able to produce atmospheric simulations/forecasts at different resolutions, for any period of time and in any region of the globe.


2009 ◽  
Vol 9 (20) ◽  
pp. 7737-7751 ◽  
Author(s):  
M. M. Kvalevåg ◽  
G. Myhre ◽  
C. E. Lund Myhre

Abstract. Human activity influences a wide range of components that affect the surface UV radiation levels, among them ozone at high latitudes. We calculate the effect of human-induced changes in the surface erythemally weighted ultra-violet radiation (UV-E) since 1750. We compare results from a radiative transfer model to surface UV-E radiation for year 2000 derived by satellite observations (from Total Ozone Mapping Spectroradiometer) and to ground based measurements at 14 sites. The model correlates well with the observations; the correlation coefficients are 0.97 and 0.98 for satellite and ground based measurements, respectively. In addition to the effect of changes in ozone, we also investigate the effect of changes in SO2, NO2, the direct and indirect effects of aerosols, albedo changes and aviation-induced contrails and cirrus. The results show an increase of surface UV-E in polar regions, most strongly in the Southern Hemisphere. Furthermore, our study also shows an extensive surface UV-E reduction over most land areas; a reduction up to 20% since 1750 is found in some industrialized regions. This reduction in UV-E over the industrial period is particularly large in highly populated regions.


2011 ◽  
Vol 4 (3) ◽  
pp. 723-757 ◽  
Author(s):  
◽  
N. Bellouin ◽  
W. J. Collins ◽  
I. D. Culverwell ◽  
P. R. Halloran ◽  
...  

Abstract. We describe the HadGEM2 family of climate configurations of the Met Office Unified Model, MetUM. The concept of a model "family" comprises a range of specific model configurations incorporating different levels of complexity but with a common physical framework. The HadGEM2 family of configurations includes atmosphere and ocean components, with and without a vertical extension to include a well-resolved stratosphere, and an Earth-System (ES) component which includes dynamic vegetation, ocean biology and atmospheric chemistry. The HadGEM2 physical model includes improvements designed to address specific systematic errors encountered in the previous climate configuration, HadGEM1, namely Northern Hemisphere continental temperature biases and tropical sea surface temperature biases and poor variability. Targeting these biases was crucial in order that the ES configuration could represent important biogeochemical climate feedbacks. Detailed descriptions and evaluations of particular HadGEM2 family members are included in a number of other publications, and the discussion here is limited to a summary of the overall performance using a set of model metrics which compare the way in which the various configurations simulate present-day climate and its variability.


2014 ◽  
Vol 10 (2) ◽  
pp. 697-713 ◽  
Author(s):  
G. Le Hir ◽  
Y. Teitler ◽  
F. Fluteau ◽  
Y. Donnadieu ◽  
P. Philippot

Abstract. During the Archaean, the Sun's luminosity was 18 to 25% lower than the present day. One-dimensional radiative convective models (RCM) generally infer that high concentrations of greenhouse gases (CO2, CH4) are required to prevent the early Earth's surface temperature from dropping below the freezing point of liquid water and satisfying the faint young Sun paradox (FYSP, an Earth temperature at least as warm as today). Using a one-dimensional (1-D) model, it was proposed in 2010 that the association of a reduced albedo and less reflective clouds may have been responsible for the maintenance of a warm climate during the Archaean without requiring high concentrations of atmospheric CO2 (pCO2). More recently, 3-D climate simulations have been performed using atmospheric general circulation models (AGCM) and Earth system models of intermediate complexity (EMIC). These studies were able to solve the FYSP through a large range of carbon dioxide concentrations, from 0.6 bar with an EMIC to several millibars with AGCMs. To better understand this wide range in pCO2, we investigated the early Earth climate using an atmospheric GCM coupled to a slab ocean. Our simulations include the ice-albedo feedback and specific Archaean climatic factors such as a faster Earth rotation rate, high atmospheric concentrations of CO2 and/or CH4, a reduced continental surface, a saltier ocean, and different cloudiness. We estimated full glaciation thresholds for the early Archaean and quantified positive radiative forcing required to solve the FYSP. We also demonstrated why RCM and EMIC tend to overestimate greenhouse gas concentrations required to avoid full glaciations or solve the FYSP. Carbon cycle–climate interplays and conditions for sustaining pCO2 will be discussed in a companion paper.


2014 ◽  
Vol 27 (20) ◽  
pp. 7725-7752 ◽  
Author(s):  
Anthony J. Baran ◽  
Peter Hill ◽  
Kalli Furtado ◽  
Paul Field ◽  
James Manners

Abstract A new coupled cloud physics–radiation parameterization of the bulk optical properties of ice clouds is presented. The parameterization is consistent with assumptions in the cloud physics scheme regarding particle size distributions (PSDs) and mass–dimensional relationships. The parameterization is based on a weighted ice crystal habit mixture model, and its bulk optical properties are parameterized as simple functions of wavelength and ice water content (IWC). This approach directly couples IWC to the bulk optical properties, negating the need for diagnosed variables, such as the ice crystal effective dimension. The parameterization is implemented into the Met Office Unified Model Global Atmosphere 5.0 (GA5) configuration. The GA5 configuration is used to simulate the annual 20-yr shortwave (SW) and longwave (LW) fluxes at the top of the atmosphere (TOA), as well as the temperature structure of the atmosphere, under various microphysical assumptions. The coupled parameterization is directly compared against the current operational radiation parameterization, while maintaining the same cloud physics assumptions. In this experiment, the impacts of the two parameterizations on the SW and LW radiative effects at TOA are also investigated and compared against observations. The 20-yr simulations are compared against the latest observations of the atmospheric temperature and radiative fluxes at TOA. The comparisons demonstrate that the choice of PSD and the assumed ice crystal shape distribution are as important as each other. Moreover, the consistent radiation parameterization removes a long-standing tropical troposphere cold temperature bias but slightly warms the southern midlatitudes by about 0.5 K.


2018 ◽  
Vol 7 (3) ◽  
pp. 6657
Author(s):  
Atika RADID ◽  
Karim RHOFIR

Generally, chemical reactions from atmospheric chemistry models are described by a strongly coupled, stiff and nonlinear system of ordinary differential equations, which requires a good numerical solver. Several articles published about the solvers of chemical equations, during the numerical simulation, indicate that one renders the concentration null when it becomes negative. In order to preserve the positivity of the exact solutions, recent works have proposed a new solver called Modified-Backward-Euler (MBE). To improve this solver, we propose in this paper an iterative numerical scheme witch is better fitted to stiff problems. This new approach, called Iterative-Modified-Backward-Euler (IMBE), is based on iterative solution of the P-L structure of the implicit nonlinear ordinary differential equations on each time step. The efficiency of the iteration process is increased by using the Gauss and Successive-Over-Relaxation (SOR). In the case of fast/slow chemical kinetic reactions, we proposed an other variant called Iterative-Quasi-Steady-State-Approximation (IQSSA). The numerical exploration of stiff test problem shows clearly that this formalism is applicable to a wide range of chemical kinetics problems and give a good approximation compared to the recent solver. The numerical procedures give reasonable accurate solutions when compared to exact solution.Generally, chemical reactions from atmospheric chemistry models are described by a strongly coupled, stiff and nonlinear system of ordinary differential equations, which requires a good numerical solver. Several articles published about the solvers of chemical equations, during the numerical simulation, indicate that one renders the concentration null when it becomes negative. In order to preserve the positivity of the exact solutions, recent works have proposed a new solver called Modified-Backward-Euler (MBE). To improve this solver, we propose in this paper an iterative numerical scheme witch is better fitted to stiff problems. This new approach, called Iterative-Modified-Backward-Euler (IMBE), is based on iterative solution of the P-L structure of the implicit nonlinear ordinary differential equations on each time step. The efficiency of the iteration process is increased by using the Gauss and Successive-Over-Relaxation (SOR). In the case of fast/slow chemical kinetic reactions, we proposed an other variant called Iterative-Quasi-Steady-State-Approximation (IQSSA). The numerical exploration of stiff test problem shows clearly that this formalism is applicable to a wide range of chemical kinetics problems and give a good approximation compared to the recent solver. The numerical procedures give reasonable accurate solutions when compared to exact solution.


2015 ◽  
Vol 28 (2) ◽  
pp. 135-149 ◽  
Author(s):  
U. Falk ◽  
H. Gieseke ◽  
F. Kotzur ◽  
M. Braun

AbstractChanges of glaciers and snow cover in polar regions affect a wide range of physical and ecosystem processes on land and in the adjacent marine environment. In this study, we investigated the potential of 11-day repeat high-resolution satellite image time series from the TerraSAR-X mission to derive glaciological and hydrological parameters on King George Island, Antarctica, between 25 October 2010 and 19 April 2011. The spatial pattern and temporal evolution of snow cover extent on ice-free areas can be monitored using multi-temporal coherence images. Synthetic aperture radar (SAR) coherence is used to map glacier extent of land-terminating glaciers with an average accuracy of 25 m. Multi-temporal SAR colour composites identify the position of the late summer snow line at ~220 m a.s.l. Glacier surface velocities are obtained from intensity feature-tracking. Surface velocities near the calving front of Fourcade Glacier were up to 1.8±0.01 m d-1. Using an intercept theorem based on fundamental geometric principles together with differential GPS field measurements, the ice discharge of Fourcade Glacier was estimated at 20 700±5500 m3 d-1 (corresponding to ~19±5 kt d-1). The rapidly changing surface conditions on King George Island and the lack of high-resolution digital elevation models for the region remain restrictions for the applicability of SAR data and the precision of derived products. Supplemental data are available at http://dx.doi.org/10.1594/PANGAEA.853954.


2016 ◽  
Vol 9 (8) ◽  
pp. 3817-3836 ◽  
Author(s):  
Naruki Hiranuma ◽  
Ottmar Möhler ◽  
Gourihar Kulkarni ◽  
Martin Schnaiter ◽  
Steffen Vogt ◽  
...  

Abstract. Separation of particles that play a role in cloud activation and ice nucleation from interstitial aerosols has become necessary to further understand aerosol-cloud interactions. The pumped counterflow virtual impactor (PCVI), which uses a vacuum pump to accelerate the particles and increase their momentum, provides an accessible option for dynamic and inertial separation of cloud elements. However, the use of a traditional PCVI to extract large cloud hydrometeors is difficult mainly due to its small cut-size diameters (< 5 µm). Here, for the first time we describe a development of an ice-selecting PCVI (IS-PCVI) to separate ice in controlled mixed-phase cloud system based on the particle inertia with the cut-off diameter  ≥  10 µm. We also present its laboratory application demonstrating the use of the impactor under a wide range of temperature and humidity conditions. The computational fluid dynamics simulations were initially carried out to guide the design of the IS-PCVI. After fabrication, a series of validation laboratory experiments were performed coupled with the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) expansion cloud simulation chamber. In the AIDA chamber, test aerosol particles were exposed to the ice supersaturation conditions (i.e., RHice > 100 %), where a mixture of droplets and ice crystals was formed during the expansion experiment. In parallel, the flow conditions of the IS-PCVI were actively controlled, such that it separated ice crystals from a mixture of ice crystals and cloud droplets, which were of diameter  ≥  10 µm. These large ice crystals were passed through the heated evaporation section to remove the water content. Afterwards, the residuals were characterized with a suite of online and offline instruments downstream of the IS-PCVI. These results were used to assess the optimized operating parameters of the device in terms of (1) the critical cut-size diameter, (2) the transmission efficiency and (3) the counterflow-to-input flow ratio. Particle losses were characterized by comparing the residual number concentration to the rejected interstitial particle number concentration. Overall results suggest that the IS-PCVI enables inertial separation of particles with a volume-equivalent particle size in the range of  ~ 10–30 µm in diameter with small inadvertent intrusion (~  5 %) of unwanted particles.


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