scholarly journals Optical properties of laboratory grown sea ice doped with light absorbing impurities (black carbon)

2017 ◽  
Author(s):  
Amelia A. Marks ◽  
Maxim L. Lamare ◽  
Martin D. King

Abstract. Sea ice radiative-transfer models are of great importance for prediction of future sea ice trends but they are limited by uncertainty in models and requirement for evaluation of modelled irradiance data against measured irradiance data. Presented here are the first results from the Royal Holloway sea ice simulator used to evaluate the output of the TUV-snow radiative-transfer model against the optical properties from the simulated sea ice. The sea ice simulator creates a realistic sea ice environment where both optical (reflectance and light penetration depth (e-folding depth)) and physical (temperature, salinity, density) properties of a ∼ 30 cm thick sea ice can be monitored and measured. Using albedo and e-folding depth data measured from simulated sea ice, scattering and absorption cross-sections of the ice are derived using the TUV-snow model. Absorption cross-sections for the ice are highly wavelength dependent, suggesting the addition of a further absorbing impurity in the ice matching the absorption spectrum of algae. Scattering cross-sections were wavelength independent with values ranging from 0.012 and 0.032 cm2 kg−1 for different ice created in the simulator. Reflectance and light penetration depth (e-folding depth) of sea ice is calculated from the derived values of the scattering and absorption cross-section using the TUV-snow model within error of the experiment. The model is also shown to replicate ice optical properties for sea ice with an extra layer doped with black carbon, well within error of the experiment. Particulate black carbon at mass ratios of 75, 150 and 300 ng g−1 in a 5 cm ice layer lowers the albedo by 97 %, 90 %, and 79 % compared to clean ice at a wavelength of 500 nm.

2017 ◽  
Vol 11 (6) ◽  
pp. 2867-2881 ◽  
Author(s):  
Amelia A. Marks ◽  
Maxim L. Lamare ◽  
Martin D. King

Abstract. Radiative-transfer calculations of the light reflectivity and extinction coefficient in laboratory-generated sea ice doped with and without black carbon demonstrate that the radiative-transfer model TUV-snow can be used to predict the light reflectance and extinction coefficient as a function of wavelength. The sea ice is representative of first-year sea ice containing typical amounts of black carbon and other light-absorbing impurities. The experiments give confidence in the application of the model to predict albedo of other sea ice fabrics. Sea ices,  ∼  30 cm thick, were generated in the Royal Holloway Sea Ice Simulator ( ∼  2000 L tanks) with scattering cross sections measured between 0.012 and 0.032 m2 kg−1 for four ices. Sea ices were generated with and without  ∼  5 cm upper layers containing particulate black carbon. Nadir reflectances between 0.60 and 0.78 were measured along with extinction coefficients of 0.1 to 0.03 cm−1 (e-folding depths of 10–30 cm) at a wavelength of 500 nm. Values were measured between light wavelengths of 350 and 650 nm. The sea ices generated in the Royal Holloway Sea Ice Simulator were found to be representative of natural sea ices. Particulate black carbon at mass ratios of  ∼  75,  ∼  150 and  ∼  300 ng g−1 in a 5 cm ice layer lowers the albedo to 97, 90 and 79 % of the reflectivity of an undoped clean sea ice (at a wavelength of 500 nm).


2014 ◽  
Vol 8 (5) ◽  
pp. 1625-1638 ◽  
Author(s):  
A. A. Marks ◽  
M. D. King

Abstract. The optical properties of snow/sea ice vary with age and by the processes they were formed, giving characteristic types of snow and sea ice. The response of albedo and light penetration depth (e-folding depth) to increasing mass ratio of black carbon is shown to depend on the snow and sea ice type and the thickness of the snow or sea ice. The response of albedo and e-folding depth of three different types of snow (cold polar snow, wind-packed snow and melting snow) and three sea ice (multi-year ice, first-year ice and melting sea ice) to increasing mass ratio of black carbon is calculated using a coupled atmosphere–snow/sea ice radiative-transfer model (TUV-snow), over the optical wavelengths of 300–800 nm. The snow and sea ice types are effectively defined by a scattering cross-section, density and asymmetry parameter. The relative change in albedo and e-folding depth of each of the three snow and three sea ice types with increasing mass ratio of black carbon is considered relative to a base case of 1 ng g−1 of black carbon. The relative response of each snow and sea ice type is intercompared to examine how different types of snow and sea ice respond relative to each other. The relative change in albedo of a melting snowpack is a factor of four more responsive to additions of black carbon compared to cold polar snow over a black carbon increase from 1 to 50 ng g−1, while the relative change in albedo of a melting sea ice is a factor of two more responsive to additions of black carbon compared to multi-year ice for the same increase in mass ratio of black carbon. The response of e-folding depth is effectively not dependent on snow/sea ice type. The albedo of sea ice is more responsive to increasing mass ratios of black carbon than snow.


2014 ◽  
Vol 8 (1) ◽  
pp. 1023-1056
Author(s):  
A. A. Marks ◽  
M. D. King

Abstract. The optical properties of snow/sea ice vary with age and by the processes they were formed, giving characteristic types of snow and sea ice. The response of albedo and light penetration depth (e-folding depth) to increasing mass-ratio of black carbon is shown to depend on the snow and sea ice type and the thickness of the snow or sea ice. The response of albedo and e-folding depth of three different types of snow (cold polar snow, windpacked snow and melting snow) and three sea ice (multi-year ice, first-year ice and melting sea ice) to increasing black carbon is calculated using a coupled atmosphere–snow/sea ice radiative-transfer model (TUV-snow), over the optical wavelengths of 300–700 nm. The snow and sea ice types are defined by a scattering-cross section, density and asymmetry parameter. The relative change in albedo of a melting snowpack is a factor of four more responsive to additions of black carbon compared to cold polar snow over a black carbon increase from 1 to 50 ng g−1. While the relative change in albedo of a melting sea ice is a factor of two more responsive to additions of black carbon compared to multi-year ice for the same black carbon mass-ratio increase. The response of e-folding depth is effectively not dependent on snow/sea ice type. The albedo of sea ice is more responsive to increased mass-ratios of black carbon than snow.


2014 ◽  
Vol 7 (5) ◽  
pp. 2503-2516 ◽  
Author(s):  
K. Klingmüller ◽  
B. Steil ◽  
C. Brühl ◽  
H. Tost ◽  
J. Lelieveld

Abstract. The modelling of aerosol radiative forcing is a major cause of uncertainty in the assessment of global and regional atmospheric energy budgets and climate change. One reason is the strong dependence of the aerosol optical properties on the mixing state of aerosol components, such as absorbing black carbon and, predominantly scattering sulfates. Using a new column version of the aerosol optical properties and radiative-transfer code of the ECHAM/MESSy atmospheric-chemistry–climate model (EMAC), we study the radiative transfer applying various mixing states. The aerosol optics code builds on the AEROPT (AERosol OPTical properties) submodel, which assumes homogeneous internal mixing utilising the volume average refractive index mixing rule. We have extended the submodel to additionally account for external mixing, partial external mixing and multilayered particles. Furthermore, we have implemented the volume average dielectric constant and Maxwell Garnett mixing rule. We performed regional case studies considering columns over China, India and Africa, corroborating much stronger absorption by internal than external mixtures. Well-mixed aerosol is a good approximation for particles with a black-carbon core, whereas particles with black carbon at the surface absorb significantly less. Based on a model simulation for the year 2005, we calculate that the global aerosol direct radiative forcing for homogeneous internal mixing differs from that for external mixing by about 0.5 W m−2.


2019 ◽  
Vol 13 (8) ◽  
pp. 2169-2187 ◽  
Author(s):  
Francois Tuzet ◽  
Marie Dumont ◽  
Laurent Arnaud ◽  
Didier Voisin ◽  
Maxim Lamare ◽  
...  

Abstract. Light-absorbing particles (LAPs) such as black carbon or mineral dust are some of the main drivers of snow radiative transfer. Small amounts of LAPs significantly increase snowpack absorption in the visible wavelengths where ice absorption is particularly weak, impacting the surface energy budget of snow-covered areas. However, linking measurements of LAP concentration in snow to their actual radiative impact is a challenging issue which is not fully resolved. In the present paper, we point out a new method based on spectral irradiance profile (SIP) measurements which makes it possible to identify the radiative impact of LAPs on visible light extinction in homogeneous layers of the snowpack. From this impact on light extinction it is possible to infer LAP concentrations present in each layer using radiative transfer theory. This study relies on a unique dataset composed of 26 spectral irradiance profile measurements in the wavelength range 350–950 nm with concomitant profile measurements of snow physical properties and LAP concentrations, collected in the Alps over two snow seasons in winter and spring conditions. For 55 homogeneous snow layers identified in our dataset, the concentrations retrieved from SIP measurements are compared to chemical measurements of LAP concentrations. A good correlation is observed for measured concentrations higher than 5 ng g−1 (r2=0.81) despite a clear positive bias. The potential causes of this bias are discussed, underlining a strong sensitivity of our method to LAP optical properties and to the relationship between snow microstructure and snow optical properties used in the theory. Additional uncertainties such as artefacts in the measurement technique for SIP and chemical contents along with LAP absorption efficiency may explain part of this bias. In addition, spectral information on LAP absorption can be retrieved from SIP measurements. We show that for layers containing a unique absorber, this absorber can be identified in some cases (e.g. mineral dust vs. black carbon). We also observe an enhancement of light absorption between 350 and 650 nm in the presence of liquid water in the snowpack, which is discussed but not fully elucidated. A single SIP acquisition lasts approximately 1 min and is hence much faster than collecting a profile of chemical measurements. With the recent advances in modelling LAP–snow interactions, our method could become an attractive alternative to estimate vertical profiles of LAP concentrations in snow.


2021 ◽  
Vol 21 (17) ◽  
pp. 12989-13010
Author(s):  
Baseerat Romshoo ◽  
Thomas Müller ◽  
Sascha Pfeifer ◽  
Jorge Saturno ◽  
Andreas Nowak ◽  
...  

Abstract. The formation of black carbon fractal aggregates (BCFAs) from combustion and subsequent ageing involves several stages resulting in modifications of particle size, morphology, and composition over time. To understand and quantify how each of these modifications influences the BC radiative forcing, the optical properties of BCFAs are modelled. Owing to the high computational time involved in numerical modelling, there are some gaps in terms of data coverage and knowledge regarding how optical properties of coated BCFAs vary over the range of different factors (size, shape, and composition). This investigation bridged those gaps by following a state-of-the-art description scheme of BCFAs based on morphology, composition, and wavelength. The BCFA optical properties were investigated as a function of the radius of the primary particle (ao), fractal dimension (Df), fraction of organics (forganics), wavelength (λ), and mobility diameter (Dmob). The optical properties are calculated using the multiple-sphere T-matrix (MSTM) method. For the first time, the modelled optical properties of BC are expressed in terms of mobility diameter (Dmob), making the results more relevant and relatable for ambient and laboratory BC studies. Amongst size, morphology, and composition, all the optical properties showed the highest variability with changing size. The cross sections varied from 0.0001 to 0.1 µm2 for BCFA Dmob ranging from 24 to 810 nm. It has been shown that MACBC and single-scattering albedo (SSA) are sensitive to morphology, especially for larger particles with Dmob > 100 nm. Therefore, while using the simplified core–shell representation of BC in global models, the influence of morphology on radiative forcing estimations might not be adequately considered. The Ångström absorption exponent (AAE) varied from 1.06 up to 3.6 and increased with the fraction of organics (forganics). Measurement results of AAE ≫ 1 are often misinterpreted as biomass burning aerosol, it was observed that the AAE of purely black carbon particles can be ≫ 1 in the case of larger BC particles. The values of the absorption enhancement factor (Eλ) via coating were found to be between 1.01 and 3.28 in the visible spectrum. The Eλ was derived from Mie calculations for coated volume equivalent spheres and from MSTM for coated BCFAs. Mie-calculated enhancement factors were found to be larger by a factor of 1.1 to 1.5 than their corresponding values calculated from the MSTM method. It is shown that radiative forcings are highly sensitive to modifications in morphology and composition. The black carbon radiative forcing ΔFTOA (W m−2) decreases up to 61 % as the BCFA becomes more compact, indicating that global model calculations should account for changes in morphology. A decrease of more than 50 % in ΔFTOA was observed as the organic content of the particle increased up to 90 %. The changes in the ageing factors (composition and morphology) in tandem result in an overall decrease in the ΔFTOA. A parameterization scheme for optical properties of BC fractal aggregates was developed, which is applicable for modelling, ambient, and laboratory-based BC studies. The parameterization scheme for the cross sections (extinction, absorption, and scattering), single-scattering albedo (SSA), and asymmetry parameter (g) of pure and coated BCFAs as a function of Dmob were derived from tabulated results of the MSTM method. Spanning an extensive parameter space, the developed parameterization scheme showed promisingly high accuracy up to 98 % for the cross sections, 97 % for single-scattering albedos (SSAs), and 82 % for the asymmetry parameter (g).


Nanomaterials ◽  
2022 ◽  
Vol 12 (1) ◽  
pp. 151
Author(s):  
Ivan D. Skurlov ◽  
Wenxu Yin ◽  
Azat O. Ismagilov ◽  
Anton N. Tcypkin ◽  
Haohang Hua ◽  
...  

Metal halide perovskite nanocrystals (NCs) attract much attention for light-emitting applications due to their exceptional optical properties. More recently, perovskite NCs have begun to be considered a promising material for nonlinear optical applications. Numerous strategies have recently been developed to improve the properties of metal halide perovskite NCs. Among them, B-site doping is one of the most promising ways to enhance their brightness and stability. However, there is a lack of study of the influence of B-site doping on the nonlinear optical properties of inorganic perovskite NCs. Here, we demonstrate that Cd2+ doping simultaneously improves both the linear (higher photoluminescence quantum yield, larger exciton binding energy, reduced trap states density, and faster radiative recombination) and nonlinear (higher two- and three-photon absorption cross-sections) optical properties of CsPbBr3 NCs. Cd2+ doping results in a two-photon absorption cross-section, reaching 2.6 × 106 Goeppert-Mayer (GM), which is among the highest reported for CsPbBr3 NCs.


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