Mie Calculations Research Articles

Auto Aligning, Error-Compensated Broadband Collimated Transmission Spectroscopy.

Broadband spectral measurements of the ballistic transmission of scattering samples are challenging. The presented work shows an approach that includes a broadband system and an automated adjustment unit for compensation of angular distortions caused by non-plane-parallel samples. The limits of the system in terms of optimal transmission and detected forward scattering influenced by the scattering phase function are investigated. We built and validated a setup that measures the collimated transmission signal in a spectral range from 300 nm to 2150 nm. The system was validated using polystyrene spheres and Mie calculations. The limits of the system in terms of optimal transmission and detected forward scattering were researched. The optimal working parameters of the system, analyzed by simulations using the Monte Carlo method, show that the transmission should be larger than 10% and less than 90% to allow for a reliable measurement with acceptable errors caused by noise and systematic errors of the system. The optimal transmission range is between 25% and 50%. We show that the phase function is important when considering the accuracy of the measurement. For strongly forward-scattering samples, errors of up to 80% can be observed, even for a very small numerical aperture of 6.6·10-4, as used in our experimental system. We also show that errors increase with optical thickness as the ballistic transmission decreases and the multiscattered fraction increases. In addition, errors caused by multiple reflections in the sample layer were analyzed and also classified as relevant for classical absorption spectroscopy.

Light Scattering Measurements of KCl Particles as an Exoplanet Cloud Analog

Salt clouds are predicted to be common on warm exoplanets, but their optical properties are uncertain. The Exoplanet Cloud Ensemble Scattering System (ExCESS), a new apparatus to measure the scattering intensity and degree of linear polarization for an ensemble of particles, is introduced here and used to study the light scattering properties of KCl cloud analogs. ExCESS illuminates particles with a polarized laser beam (532 nm) and uses a photomultiplier tube detector to sweep the plane of illumination. Scattering measurements for KCl particles were collected for three size distributions representative of modeled clouds for the warm exoplanet GJ 1214b. Our measurements show that Lorenz–Mie calculations, commonly used to estimate the light scattering properties of assumedly spherical cloud particles, offer an inaccurate depiction of cubic and cuboid KCl particles. All of our measurements indicate that Lorenz–Mie scattering overestimates the backscattering intensity of our cloud analogs and incorrectly predicts the scattering at mid-phase angles (∼90°) and the preferential polarization state of KCl scattered light. Our results align with the general scattering properties of nonspherical particles and underscore the importance of further understanding the effects that such particles will have on radiative transfer models of exoplanet atmospheres and reflected light observations of exoplanets by the upcoming Nancy Grace Roman Space Telescope and Habitable Worlds Observatory.

A Methylene Blue/Sodium Sulfinate Photo‐Initiating System for the Red‐Light Emulsion Photopolymerization of Methyl Methacrylate

AbstractThe emulsion photopolymerization of methyl methacrylate (MMA) using red light is reported. The synthesis of poly(methyl methacrylate) (PMMA) latexes is initiated by irradiation of a new, very efficient red‐absorbing methylene blue (MB)/sodium para‐toluenesulfinate (NapTS) system in the red region (660 nm). Visible, and especially red light penetrates the dispersed medium imposed by the emulsion process better than ultra‐violet photons (UVs). However, emulsion photopolymerizations require the development of fully water‐soluble initiating systems activable by red light, which is still hugely challenging because red photons are much less energetic, therefore generally lead to less efficient photochemical processes. The influence of the surfactant concentration and the solids content is examined over particle sizes and polymerization kinetics. The polymerizations work for solids contents between 10 and 25 wt%, with narrowly distributed particles of average sizes ranging from 40 to 65 nm. Calculations of Mie scattering support the observation that at a given wavelength the larger the particles the lower the penetration. All latexes obtained are slightly blue, which are traced to the regeneration of MB when the latexes are exposed to dioxygen. The dye regeneration enables the reactivation of the photopolymerization process.

MieAI: a neural network for calculating optical properties of internally mixed aerosol in atmospheric models

Aerosols influence weather and climate by interacting with radiation through absorption and scattering. These effects heavily rely on the optical properties of aerosols, which are mainly governed by attributes such as morphology, size distribution, and chemical composition. These attributes undergo continuous changes due to chemical reactions and aerosol micro-physics, resulting in significant spatio-temporal variations. Most atmospheric models struggle to incorporate this variability because they use pre-calculated tables to handle aerosol optics. This offline approach often leads to substantial errors in estimating the radiative impacts of aerosols along with posing significant computational burdens. To address this challenge, we introduce a computationally efficient and robust machine learning approach called MieAI. It allows for relatively inexpensive calculation of the optical properties of internally mixed aerosols with a log-normal size distribution. Importantly, MieAI fully incorporates the variability in aerosol chemistry and microphysics. Our evaluation of MieAI against traditional Mie calculations, using number concentrations from the ICOsahedral Nonhydrostatic model with Aerosol and Reactive Trace gases (ICON-ART) simulations, demonstrates that MieAI exhibits excellent predictive accuracy for aerosol optical properties. MieAI achieves this with errors well within 10%, and it operates more than 1000 times faster than the benchmark approach of Mie calculations. Due to its generalized nature, the MieAI approach can be implemented in any chemistry transport model which represents aerosol size distribution in the form of log-normally distributed internally mixed modes. This advancement has the potential to replace frequently employed look-up tables and plays a substantial role in the ongoing attempts to reduce uncertainties in estimating aerosol radiative forcing.

Targeted color design of silver-gold alloy nanoparticles.

This research article focuses on the targeted color design of silver-gold alloy nanoparticles (NPs), employing a multivariate optimization approach. NP synthesis involves interconnected process parameters, making independent variation challenging. Data-based property-process relationships are established to optimize optical properties effectively. We define a color target, employ a green chemical co-reduction method at room temperature and optimize process parameters accordingly. The CIEL*a*b* color space (Commission Internationale de l'Éclairage - International Commission on Illumination) and Euclidean distances facilitate accurate color matching to establish the property-process relationship. Concurrently, theoretical Mie calculations explore the structure-property relationship across particle sizes, concentrations, and molar gold contents. The theoretically optimal structure agrees very well with experimental particle structures at the property-process relationship's optimum. The data-driven property-process relationship provides valuable insights into the formation mechanism of a complex particle system, sheds light on the role of relevant process parameters and allows to evaluate the practically available property space. Model validation beyond the original grid demonstrates its robustness, yielding colors close to the target. Additionally, Design of Experiments (DoE) methods reduce experimental work by threefold with slight accuracy trade-offs. Our novel methodology for targeted color design demonstrates how data-based methods can be utilized alongside structure-property relationships to unravel property-process relationships in the design of complex nanoparticle systems and paves the way for future developments in targeted property design.

Raman lidar-derived optical and microphysical properties of ice crystals within thin Arctic clouds during PARCS campaign

Abstract. Cloud observations in the Arctic are still rare, which requires innovative observation techniques to assess ice crystal properties. We present an original approach using the Raman lidar measurements applied to a case study in northern Scandinavia. The vertical profiles of the optical properties, the effective radius of ice crystals and ice water content (IWC) in Arctic semi-transparent clouds were assessed using quantitative ground-based lidar measurements at 355 nm performed from 13 to 26 May 2016 in Hammerfest (north of Norway, 70∘39′48′′ N, 23∘41′00′′ E). The field campaign was part of the Pollution in the ARCtic System (PARCS) project of the French Arctic Initiative. The presence of low-level semi-transparent clouds was noted on 16 and 17 May. The cloud base was located just above the atmospheric boundary layer where the 0 ∘C isotherm reached around 800 m above the mean sea level (a.m.s.l.). To ensure the best penetration of the laser beam into the cloud, we selected case studies with cloud optical thickness (COT) lower than 2 and out of supercooled liquid pockets. Lidar-derived multiple scattering coefficients were found to be close to 1 and ice crystal depolarization around 10 %, suggesting that ice crystals were small and had a rather spherical shape. Using Mie computations, we determine effective radii between ∼7 and 25 µm in the clouds for ice water contents between 1 and 8 mg m−3, respectively. The uncertainties regarding the effective radii and ice water content are on average 2 µm and 0.65 mg m−3, respectively.

Ephemeral Ice Clouds in the Upper Mesosphere of Venus

AbstractThe conditions in Venus' upper mesosphere at around 120 km have some similarities to the upper mesosphere of Earth and Mars where ice clouds form. Here we show, using published satellite products and numerical modeling, that the upper mesosphere of Venus can be sufficiently cold that both H2O and CO2 may condense to form particles. We show that amorphous solid water particles (ASW) are likely to nucleate both heterogeneously on meteoric smoke and also homogeneously, resulting in clouds of nano‐scaled particles at around 120 km that will occur globally. The temperatures may then become sufficiently low, below ∼90 K, that CO2 particles can nucleate on ASW particles. Given the uncertainty associated with retrievals of temperature in the upper mesosphere, it is unclear how frequently this occurs, but it could be >30% of the time poleward of 60°. Since the main component of Venus' tenuous atmosphere is CO2, any CO2 crystals that form will grow and sediment on a timescale of 10–20 min. Mie calculations show that these Venusian mesospheric clouds (VMCs) should be observable by contemporary satellite instruments, although their short lifetime means that the probability of detection is small. We suggest that VMCs are important for the redistribution of meteoric smoke and may serve as a cold‐trap, removing some water vapor from the very upper mesosphere of Venus through the growth and sedimentation of cloud particles, and possibly reducing the loss of water to space.

Ionization dynamics of sub-micrometer-sized clusters in intense ultrafast laser pulses

Sub-micrometer-sized targets are found in intense laser–cluster interaction experiments and laser-based material processing. Here, we investigate the internal field localization due to Mie scattering and its effect on ionization dynamics in sub-micrometer-sized clusters using Mie calculation and particle-in-cell simulations. As a result of intertwined processes of pulse propagation and ionization, sub-micrometer nanofocusing dominates at lower intensity and gives rise to an ionization hotspot at the rear of the targets while plasma shielding wins over at a higher intensity, stopping further rear side ionization. As ionization is often the precursor of other processes, understanding the ionization dynamics of ultrafast laser pulses with wavelength-sized nanostructure can be relevant for intense laser-cluster experiments and femtosecond laser micro-/nanomachining.

Synthetic photometry for carbon-rich giants

Context. The properties and the evolution of asymptotic giant branch (AGB) stars are strongly influenced by their mass loss through a stellar wind. This, in turn, is believed to be caused by radiation pressure due to the absorption and scattering of the stellar radiation by the dust grains formed in the atmosphere. The optical properties of dust are often estimated using the small particle limit (SPL) approximation, and it has been used frequently in modelling AGB stellar winds when performing radiation-hydrodynamics (RHD) simulations. Aims. We aim to investigate the effects of replacing the SPL approximation by detailed Mie calculations of the size-dependent opacities for grains of amorphous carbon forming in C-rich AGB star atmospheres. Methods. We performed RHD simulations for a large grid of carbon star atmosphere+wind models with different effective temperatures, luminosities, stellar masses, carbon excesses, and pulsation properties. Also, a posteriori radiative transfer calculations for many radial structures (snapshots) of these models were done, resulting in spectra and filter magnitudes. Results. We find that, when giving up the SPL approximation, the wind models become more strongly variable and more dominated by gusts, although the average mass-loss rates and outflow speeds do not change significantly; the increased radiative pressure on the dust throughout its formation zone does, however, result in smaller grains and lower condensation fractions (and thus higher gas-to-dust ratios). The photometric K magnitudes are generally brighter, but at V the effects of using size-dependent dust opacities are more complex: brighter for low mass-loss rates and dimmer for massive stellar winds. Conclusions. Given the large effects on spectra and photometric properties, it is necessary to use the detailed dust optical data instead of the simple SPL approximation in stellar atmosphere+wind modelling where dust is formed.

Stereological approach to radiative transfer in porous materials. Application to the optics of snow

Porous materials are considered as a random binary mixture of two homogeneous phases with different refractive indices; the void may be an option for one of the phases. The stereological approach has been used to formulate a system of radiative transfer equations in which the refraction/reflection by the interface between the two phases is the source of scattering. For arbitrary statistics, it is the system of integral equations with the phase chord length distributions as their kernels. For Markov statistics, it becomes the system of standard-like radiative transfer equations. For a sparse mixture, i.e. when the mean chord of one phase is much larger than that of the other, the system reduces to a single equation which is the standard radiative transfer one. Dense packing affects apparent optical properties of the medium by reducing its albedo, increasing the transmittance and shifting a position of the maximum of the light angular distribution. The model has been applied to the optics of snow. The result is a higher accuracy in retrieving the specific surface area from snow reflectance measurements when compared with the conventional method using Mie calculations. The reasons of the albedo reduction with density and of the so far successful use of the Mie solution in the optics of snow are discussed. The theory presented applies to plenty of densely packed granular media: foams, various man-made powders (food, pharmaceutic, or metal), or natural covers of planetary surfaces, such as snow, soil, sand, or regolith.

A Parameterization of Interstitial Aerosol Extinction and Its Application to Marine Cloud Brightening

Abstract Marine cloud brightening (MCB) is a geoengineering approach to counteract climate change by the deliberate seeding of sea salt aerosol particles that, once they activated to cloud droplets, directly increase cloud reflectance and hence global albedo. However, a large fraction of the seeded aerosol may remain interstitial, i.e., unactivated particles among cloud droplets. Because the consideration of interstitial aerosol optical properties usually requires computationally expensive simulations of the entire particle spectrum and direct Mie calculations, we develop a simple parameterization to be used with computationally efficient bulk and even bin cloud microphysical schemes that do not treat the unactivated aerosol explicitly. Using parcel and large-eddy simulations with highly detailed Lagrangian cloud microphysics and direct Mie calculations as a reference, we show that the parameterization captures the variability in the interstitial aerosol extinction successfully. By applying the parameterization to typical MCB cases, we find that the consideration of interstitial aerosol extinction is important for the assessment of MCB in shallow clouds with weak updrafts, in which only a small fraction of aerosol particles is activated to cloud droplets. Significance Statement The optical properties of clouds are not only determined by the number and size of cloud droplets. Unactivated aerosol particles, so-called interstitial aerosol, can contribute substantially to the optical thickness of shallow clouds with weak updrafts in aerosol-laden conditions. The consideration of interstitial aerosol optical thickness has been computationally challenging, but the new parameterization presented here allows for an efficient representation in various types of cloud models. The parameterization is shown to be an important addition for the assessment of marine cloud brightening (MCB), a potential geoengineering technique to counteract global warming by increasing the cloud albedo through the deliberate seeding of aerosol.

Localized surface plasmon resonance phenomenon in Ag/Au-WO3-x nanocomposite thin films

• Ag/Au-WO 3-x thin films prepared by radio-frequency magnetron sputtering. • The Ag/Au-WO 3-x films demonstrate localized surface plasmon resonance (LSPR) phenomenon. • Blueshift of the LSPR band in Ag-WO 3-x film. The localized surface plasmon resonance was investigated in composite thin films based on amorphous sub-stoichiometric tungsten oxide (WO 3-x ) matrix and noble metal nanoparticles, such as silver (Ag), gold (Au), and their alloy (Ag/Au). The films were prepared by radio-frequency magnetron sputtering of a combined target consisting of lemon-colored tungsten trioxide powder and Ag and/or Au pellets. It was found that the mean size of nanoparticles for all composite thin films according to the results of transmission electron microscopy is less than 5 nm. The obtained films demonstrate tunable plasmon absorption band. The position of the localized surface plasmon resonance peak was experimentally observed at 435, 494, and 582 nm for Ag-WO 3-x , Ag/Au-WO 3-x and Au-WO 3-x composite thin films, respectively. Blueshift of the localized surface plasmon resonance band in contrast with the results of Mie calculations for Ag-WO 3-x film was explained by possible formation of oxide shell on the surface of Ag nanoparticles.

Quantifying the effects of mixing state on aerosol optical properties

Abstract. Calculations of the aerosol direct effect on climate rely on simulated aerosol fields. The model representation of aerosol mixing state potentially introduces large uncertainties into these calculations, since the simulated aerosol optical properties are sensitive to mixing state. In this study, we systematically quantified the impact of aerosol mixing state on aerosol optical properties using an ensemble of 1800 aerosol populations from particle-resolved simulations as a basis for Mie calculations for optical properties. Assuming the aerosol to be internally mixed within prescribed size bins caused overestimations of aerosol absorptivity and underestimations of aerosol scattering. Together, these led to errors in the populations' single scattering albedo of up to −22.3 % with a median of −0.9 %. The mixing state metric χ proved useful in relating errors in the volume absorption coefficient, the volume scattering coefficient and the single scattering albedo to the degree of internally mixing of the aerosol, with larger errors being associated with more external mixtures. At the same time, a range of errors existed for any given value of χ. We attributed this range to the extent to which the internal mixture assumption distorted the particles' black carbon content and the refractive index of the particle coatings. Both can vary for populations with the same value of χ. These results are further evidence of the important yet complicated role of mixing state in calculating aerosol optical properties.

A dual-wavelength photothermal aerosol absorption monitor: design, calibration and performance

Abstract. There exists a lack of aerosol absorption measurement techniques with low uncertainties and without artefacts. We have developed the two-wavelength Photothermal Aerosol Absorption Monitor (PTAAM-2λ), which measures the aerosol absorption coefficient at 532 and 1064 nm. Here we describe its design, calibration and mode of operation and evaluate its applicability, limits and uncertainties. The 532 nm channel was calibrated with ∼ 1 µmol mol−1 NO2, whereas the 1064 nm channel was calibrated using measured size distribution spectra of nigrosin particles and a Mie calculation. Since the aerosolized nigrosin used for calibration was dry, we determined the imaginary part of the refractive index of nigrosin from the absorbance measurements on solid thin film samples. The obtained refractive index differed considerably from the one determined using aqueous nigrosin solution. PTAAM-2λ has no scattering artefact and features very low uncertainties: 4 % and 6 % for the absorption coefficient at 532 and 1064 nm, respectively, and 9 % for the absorption Ångström exponent. The artefact-free nature of the measurement method allowed us to investigate the artefacts of filter photometers. Both the Aethalometer AE33 and CLAP suffer from cross-sensitivity to scattering – this scattering artefact is most pronounced for particles smaller than 70 nm. We observed a strong dependence of the filter multiple scattering parameter on the particle size in the 100–500 nm range. The results from the winter ambient campaign in Ljubljana showed similar multiple scattering parameter values for ambient aerosols and laboratory experiments. The spectral dependence of this parameter resulted in AE33 reporting the absorption Ångström exponent for different soot samples with values biased 0.23–0.35 higher than the PTAAM-2λ measurement. Photothermal interferometry is a promising method for reference aerosol absorption measurements.

Polarization-based surface enhanced Raman scattering from single colloidal DNA decorated with 3 nm silicon nanoparticles

Surface enhanced Raman scattering (SERS), in which sample molecules are placed in the proximity of conducting nanostructures, subjects the molecules to intense electron oscillation (plasmon) field. The intense field, however, may cause heavy distortion and thermal damage to the molecule as well as non-separable and heavy convolution with the metal electronic structure. We utilized 3-nm red luminescent Si nanoparticles decorating the DNA molecules (drawn electrostatically) to enhance Raman scattering in solution at 532 nm. We demonstrated that the nanoparticles enhance the spectral resolution and intensity of vibrations of DNA by two orders of magnitude and reveal vibrations that are otherwise weak or forbidden. Theoretically, we conducted calculations of Mie scattering and three-dimensional finite-difference time-domain scattering and obtained the wavelength dependence of the near-field distribution from single or dimer Si particles. The simulations show moderate intensity enhancement (25–40-fold) and exciton resonances. Moreover, it shows that the near field is highly confined, extending only to 3–5 Å from the Si particle (atomic scale) compared to several nanometers for metal nanoparticles. The observed SERS-type characteristics are understood in terms of polarization-based light scattering, which is possible by the use of Si of highly reduced size for which the polarizability and exciton processes are strong. However, multilayers contribute to metal SERS, and monolayers/single molecules dominate the Si case. Weaker but highly confined, ultra-short range polarization-based scattering provides an alternative to plasmon and Mie scattering, while providing practical, straightforward interpretation of vibration printing of bio-medical species without compromising the molecular structure.

Deriving the angular response function for backscattering sensors.

We derived the angular response function (WN) for scattering sensors that automatically satisfies the normalization criterion and its corresponding weight (WT). WN's, derived for two commercial sensors, HydroScat-6 (HOBI Labs) and ECO-BB (Sea-Bird Inc.), agrees well with the Monte Carlo simulation and direct measurements. The backscattering measured for microbeads of known sizes agrees better with Mie calculation when the derived WN was applied. We deduced that the reduction of WT with increasing attenuation coefficient is related to path length attenuation and showed that this theoretically derived correction factor performs better than the default methods for the two commercial backscattering sensors. The analysis conducted in this study also leads to an estimate of uncertainty budget for the two sensors. The major uncertainty for ECO-BB is associated with its angular response function because of its wide field of view, whereas the main uncertainty for the HydrScat-6 is due to attenuation correction because of its relatively long path length.

Optical properties of coated black carbon aggregates: numerical simulations, radiative forcing estimates, and size-resolved parameterization scheme

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).

Source-specific light absorption by carbonaceous components in the complex aerosol matrix from yearly filter-based measurements

Abstract. Understanding the sources of light-absorbing organic (brown) carbon (BrC) and its interaction with black carbon (BC) and other non-refractory particulate matter (NR-PM) fractions is important for reducing uncertainties in the aerosol direct radiative forcing. In this study, we combine multiple filter-based techniques to achieve long-term, spectrally resolved, source- and species-specific atmospheric absorption closure. We determine the mass absorption efficiency (MAE) in dilute bulk solutions at 370 nm to be equal to 1.4 m2 g−1 for fresh biomass smoke, 0.7 m2 g−1 for winter-oxygenated organic aerosol (OA), and 0.13 m2 g−1 for other less absorbing OA. We apply Mie calculations to estimate the contributions of these fractions to total aerosol absorption. While enhanced absorption in the near-UV has been traditionally attributed to primary biomass smoke, here we show that anthropogenic oxygenated OA may be equally important for BrC absorption during winter, especially at an urban background site. We demonstrate that insoluble tar balls are negligible in residential biomass burning atmospheric samples of this study and thus could attribute the totality of the NR-PM absorption at shorter wavelengths to methanol-extractable BrC. As for BC, we show that the mass absorption cross-section (MAC) of this fraction is independent of its source, while we observe evidence for a filter-based lensing effect associated with the presence of NR-PM components. We find that bare BC has a MAC of 6.3 m2 g−1 at 660 nm and an absorption Ångström exponent of 0.93 ± 0.16, while in the presence of coatings its absorption is enhanced by a factor of ∼ 1.4. Based on Mie calculations of closure between observed and predicted total light absorption, we provide an indication for a suppression of the filter-based lensing effect by BrC. The total absorption reduction remains modest, ∼ 10 %–20 % at 370 nm, and is restricted to shorter wavelengths, where BrC absorption is significant. Overall, our results allow an assessment of the relative importance of the different aerosol fractions to the total absorption for aerosols from a wide range of sources and atmospheric ages. When integrated with the solar spectrum at 300–900 nm, bare BC is found to contribute around two-thirds of the solar radiation absorption by total carbonaceous aerosols, amplified by the filter-based lensing effect (with an interquartile range, IQR, of 8 %–27 %), while the IQR of the contributions by particulate BrC is 6 %–13 % (13 %–20 % at the rural site during winter). Future studies that will directly benefit from these results include (a) optical modelling aiming at understanding the absorption profiles of a complex aerosol composed of BrC, BC and lensing-inducing coatings; (b) source apportionment aiming at understanding the sources of BC and BrC from the aerosol absorption profiles; (c) global modelling aiming at quantifying the most important aerosol absorbers.

Optical density inferences in aqueous solution with embedded micro/nano bubbles: A reminder for the emerging green bubble cleantech

As an environmental friendly cleantech, micro/nano bubbles (MNBs) have been increasingly used for pollution control in cleaner production and water renewability improvement, and many works used optical density (OD) as proxy for the concentration of chemical/biological substances in liquid samples. This study reported that MNBs induced considerable light scattering and impacted the measured OD of liquid samples. The experimental results showed that bubble aeration increased the OD at wavelengths of 300–600 nm by 0.14–0.50 in commonly used bio-cultural medium and deionized water. The scattered light that fell outside the effective forward range increased the OD, and this increase was dependent on the bubble size and light wavelength. The Mie calculations showed that the scattering of smaller bubble is stronger and results in more OD increase. By defining the OD deviation <0.01, the critical thresholds of bubble size were calculated using the Kepler conjecture and Beer-Lambert’s law. For the commonly used wavelength 600 nm, the OD increase can be neglected only for bubbles with diameter >263 μm in water. The finite-difference time-domain simulation illustrated the highly nonuniform electric field near the bubble, and verified the higher scattering efficiencies at shorter wavelength. De-bubbling samples from MNB systems via short-term sonication eliminated light scattering. Findings from this work delineated the optical properties of MNBs, highlighted resulting impact on optical measurement and proposed a de-bubbling method in water treatment.

Comparing multifractal characteristics of soil particle size distributions calculated by Mie and Fraunhofer models from laser diffraction measurements

Particle size distribution (PSD) is a basic soil property, closely related to main soil physical and chemical attributes. Soil PSD determined by laser diffraction (LD) may provide additional information to soil texture determined by traditional methods. In turn, LD may be implemented using either Mie or Fraunhofer calculation methods, based on different assumptions. The multifractal approach has been demonstrated to be useful for characterizing the inner structure of soil PSD. We analysed the PSDs of 18 soil horizons sampled on the most characteristic soil types from Argentina with a wide range of textural classes, from clayey to sandy, mainly developed over loess material. Our aims were to assess the multifractality between PSDs computed using either Mie scattering or Fraunhofer diffraction models, and to compare the scaling properties and multifractal behavior of PSDs from soils with contrasting textures. Fraunhofer model provided PSD curves, which were shifted toward coarser particles compared to those obtained with Mie model. Regardless calculation method, all the PSDs studied displayed a well-defined multifractal structure, as shown by singularity, f(α) versus α, and by Rènyi spectra, Dqvs q. Moreover, all singularity spectra were strong asymmetric, right deviating curves, which is consistent with a greater heterogeneity of the low values of volume frequencies for all the PSDs analysed. Soil PSDs computed by Fraunhofer model showed higher asymmetry than those computed by Mie model for 16 out of 18 horizons studied; this suggests that scaling heterogeneity mainly depends on the support length, which is larger for the PSDs computed by Mie. In addition, other features of the PSDs stemming from soil processes such as weathering intensity of loess materials may also influence multifractality. Stronger correlations were found between multifractal parameters from PSDs calculated by the two models for the most positive q moments of singularity and Renyi spectra, i.e. α10, D10, than for those gathered from the central and negative q moments. The entropy dimension, D1, significantly (P<0.05) increased with increasing clay content, in contrast to previous findings; this may be due either to differences in the inner structure of various PSD data sets compared, or to shortcomings of standard PSD measurement and calculation procedures.