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At least 19 records

Haze–cloud correlations mediated by supersaturation fluctuations

Atmospheric aerosol particles that contain water-soluble components can absorb water vapor in humid environments and form either haze particles or cloud droplets, depending on supersaturation conditions. Laboratory and in situ measurements have shown that haze particles and cloud droplets often coexist and compete for available water vapor in shallow clouds and fogs, especially under polluted conditions. It is expected that more aerosol particles can form more haze particles and cloud droplets, so that the haze and cloud number concentrations are positively correlated. However, recent large-eddy simulations show that haze and cloud number concentration can be negatively correlated under extremely polluted conditions. Haze–cloud interactions across different environmental settings remain poorly understood. In this study, experiments in a convection cloud chamber with the same aerosol injection rate show that, as supersaturation forcing increases (i.e., changing from polluted to clean conditions), the covariance between haze and cloud droplet number concentration changes from negative to positive and finally to zero. Large-eddy simulations (LES) of the cloud chamber with a fixed supersaturation forcing but varying aerosol injection rates show a similar result for the haze–cloud correlation: near zero in clean, mean-supersaturation-dominated activation conditions; positive in moderate, supersaturation-fluctuation-influenced activation conditions; and negative in polluted, supersaturation-fluctuation-dominated activation conditions. A theoretical covariance framework was developed to interpret this behavior based on the relative magnitude and signs of the correlations between supersaturation and the populations of haze and cloud droplets. Significantly, experiments, LES, and theory all yield the same three-regime behavior for the sign of the haze–cloud covariance. Furthermore, our results show that the haze–cloud covariance remains robust and easily measurable, thereby providing a useful metric for regime identification in the atmosphere, improving regime-aware parameterizations, and informing aerosol interventions such as fog dispersion, rainfall enhancement, and albedo modification.

54 ENVIRONMENTAL SCIENCES↗

Simulated aging processes of black carbon and its impact during a severe winter haze event in the Beijing-Tianjin- Hebei region

Black carbon (BC) can mitigate or worsen air pollution through perturbing meteorological conditions. BC aging processes are important for the evolution of particle size, concentration, and optical properties of BC that determines its influence on the meteorology. Here we use the online coupled Weather Research and Forecasting-Chemistry (WRF-Chem) model to quantify the role of BC aging processes, including physical processes (PP) and absorption enhancements (AE), in exerting BC-induced meteorological changes and the associated feedback to PM2.5 (particulate matter less than 2.5 µm in diameter) and O3 concentrations during a severe haze event in Beijing-Tianjin-Hebei (BTH) region during 21-27 February 2014. Our results show that, compared to the simulation without the PP treatment, the simulated near-surface BC concentration and BC mass loading in BTH region is lowered by 6.6 % and 12.1 %, respectively, during the haze event with the PP included. PP increases the proportion of large-size BC (particle diameter greater than 0.312 µm) from 28 %-33 % to 59 %-64 % below 1000 m in BTH region. Both PP and AE enhance the “dome effect” of BC. With both PP and AE considered, a reduction in PBL height due to BC-PBL interaction is 116.3 m (20.7 %), compared to 75.7 m (13.5 %) without AE and 66.6 m (11.9 %) without both PP and AE. However, during this haze event, anomalous northeasterly winds are produced by the direct radiative effect of BC, which further affects the mixing and transport of aerosols. When PBL height is decreased (from 10:00 to 21:00), combining all the impacts on multiple meteorological factors, BC effect without PP and AE, without AE, and with PP and AE, respectively, increases surface concentrations of PM2.5 by 8.3 µg m-3 (6.1 % relative to the mean value), 6.1 µg m-3 (4.5 %) and 9.6 µg m-3 (7.0 %) but decreases surface O3 concentrations by 2.8 ppbv (7.4 %), 4.0 ppbv (9.0 %) and 5.0 ppbv (10.8 %) in BTH region averaged over 21-27 February 2014. Our results highlight the importance of the aging processes and absorption enhancements of BC in simulating weather and air quality.

Chen, Donglin↗

Microphysics regimes due to haze–cloud interactions: cloud oscillation and cloud collapse

Abstract. It is known that aqueous haze particles can be activated into cloud droplets in a supersaturated environment. However, haze–cloud interactions have not been fully explored, partly because haze particles are not represented in most cloud-resolving models. Here, we conduct a series of large-eddy simulations (LESs) of a cloud in a convection chamber using a haze-capable Eulerian-based bin microphysics scheme to explore haze–cloud interactions over a wide range of aerosol injection rates. Results show that the cloud is in a slow microphysics regime at low aerosol injection rates, where the cloud responds slowly to an environmental change and droplet deactivation is negligible. The cloud is in a fast microphysics regime at moderate aerosol injection rates, where the cloud responds quickly to an environmental change and haze–cloud interactions are important. More interestingly, two more microphysics regimes are observed at high aerosol injection rates due to haze–cloud interactions. Cloud oscillation is driven by the oscillation of the mean supersaturation around the critical supersaturation of aerosol due to haze–cloud interactions. Cloud collapse happens under weaker forcing of supersaturation where the chamber transfers cloud droplets to haze particles efficiently, leading to a significant decrease (collapse) in cloud droplet number concentration. One special case of cloud collapse is the haze-only regime. It occurs at extremely high aerosol injection rates, where droplet activation is inhibited, and the sedimentation of haze particles is balanced by the aerosol injection rate. Our results suggest that haze particles and their interactions with cloud droplets should be considered, especially in polluted conditions.

54 ENVIRONMENTAL SCIENCES↗

An Intercomparison of Large‐Eddy Simulations of a Convection Cloud Chamber Using Haze‐Capable Bin and Lagrangian Cloud Microphysics Schemes

Abstract Recent in situ observations show that haze particles exist in a convection cloud chamber. The microphysics schemes previously used for large‐eddy simulations of the cloud chamber could not fully resolve haze particles and the associated processes, including their activation and deactivation. Specifically, cloud droplet activation was modeled based on Twomey‐type parameterizations, wherein cloud droplets were formed when a critical supersaturation for the available cloud condensation nuclei (CCN) was exceeded and haze particles were not explicitly resolved. Here, we develop and adapt haze‐capable bin and Lagrangian microphysics schemes to properly resolve the activation and deactivation processes. Results are compared with the Twomey‐type CCN‐based bin microphysics scheme in which haze particles are not fully resolved. We find that results from the haze‐capable bin microphysics scheme agree well with those from the Lagrangian microphysics scheme. However, both schemes significantly differ from those from a CCN‐based bin microphysics scheme unless CCN recycling is considered. Haze particles from the recycling of deactivated cloud droplets can strongly enhance cloud droplet number concentration due to a positive feedback in haze‐cloud interactions in the cloud chamber. Haze particle size distributions are more realistic when considering solute and curvature effects that enable representing the complete physics of the activation process. Our study suggests that haze particles and their interactions with cloud droplets may have a strong impact on cloud properties when supersaturation fluctuations are comparable to mean supersaturation, as is the case in the cloud chamber and likely is the case in the atmosphere, especially in polluted conditions.

54 ENVIRONMENTAL SCIENCES↗

Plasmonic absorption-induced haze suppression in random scattering media

Light propagation in random scattering media is a common phenomenon in many scientific and engineering fields. Because of light-matter interaction, part of the light transmitted through a random scattering medium is diffuse and causes haze. Previous approaches to manipulate haze in random media mainly focused on regulating scattering and paid little attention to absorption. In this work, we present a comprehensive analysis of absorption-scattering coupling as well as its impact on haze in random media. We introduce the haze-absorption sensitivity (HAS) spectrum, an intrinsic property of a scattering medium that quantifies the potential of absorption-induced haze suppression. We also investigate the effect of scatterer geometry and concentration on the HAS spectrum. To experimentally demonstrate the effect of absorption in random media, we utilized the plasmonic absorption of silver and gold nanoparticles to reduce haze in a silica nanoparticle aqueous solution as the scattering medium. We showed that 15% (absolute) of haze suppression is possible by carefully choosing the optimal absorber. The experimental results closely matched the theoretical predictions. This work provides new understandings of absorption and scattering coupling in random media. The fundamental mechanisms elucidated in this work can offer new pathways for regulating haze in a variety of random scattering media.

Zhao, Lin (ORCID:000000028865859X)↗

Factors affecting relative humidity and its relationship with the long-term variation of fog-haze events in the Yangtze River Delta

Relative humidity (RH) is one of the most important parameters in the study of fog-haze. This paper first estimates the contributions of the key quantities (temperature, water vapor, air pollutant) and their combinations to the relative change of RH, and then investigates the relationships of RH with the long-term variation of haze and fog days based on the meteorological data in the Yangtze River Delta over the period 1970-2010.The main conclusions are as follows. (1) Temperature is the foremost factor influencing RH, with the effect of specific humidity and direct contribution of air pollutant being second and third. (2) RH shows a prominent descending trend in the Yangtze River Delta, due to global warming and the ‘analogous heat island effect’ (AHIE). (3) Decreasing RH was responsible for the reduction of fog days. The AHIE can explain the phenomenon in which fog days in metropolises are less than in small cities. (4) Granger causality analysis of inter-annual variation further shows that increasing aerosol loading Ganger-causes the increasing haze days, rather than meteorological parameters such as RH. High RH would enhance hygroscopic growth of particle and then suppress the planet boundary layer height (PBLH) and lead to more haze days, lower PBLH further increases aerosols and RH, this positive feedback mechanism can be established under the condition of aerosol loading being relatively stable and beyond the threshold for haze formation. (5) If aerosol emissions maintain the status quo, climate cooling would result in serious fog-haze events occurring more frequently in Yangtze River Delta. The research provide a scientific basis for understanding the influence of meteorological factors on RH and the connection between the variation of long term fog-haze days and RH under the background of climate change.

54 ENVIRONMENTAL SCIENCES↗

Flexible nanograss with highest combination of transparency and haze for optoelectronic plastic substrates

Transparent polymer substrates have recently received increased attention for various flexible optoelectronic devices. Optoelectronic applications such as solar cells and light emitting-diodes would benefit from substrates with both high transparency and high haze, which increase how much light scatters into or out of the underlying photoactive layers. In this letter, we demonstrate a new flexible nanograss plastic substrate that displays the highest combination of transparency and haze in the literature for polyethylene terephthalate (PET). Here, as opposed to other nanostructures that increase haze at the expense of transparency, our nanograss demonstrates the potential to improve both haze and transparency. Furthermore, the monolithic nanograss may be fabricated in a facile scalable maskless reactive ion etching process without the need for additional lithography or synthesis of nanostructures. Our 9 μ m height nanograss sample exhibits a transparency and haze of 92.4% and 89.4%, respectively, and our 34 μ m height nanograss displays a transparency and haze of 91.0% and 97.1%, respectively. We also performed durability experiments that demonstrate these nanostructured PET substrates are robust from bending and show similar transmission and haze values after 5000 cycles of bending.

42 ENGINEERING↗

Long-range transport impacts on surface aerosol concentrations and the contributions to haze events in China: an HTAP2 multi-model study

Haze has been severely affecting the densely populated areas in China recently. While many of the efforts have been devoted to investigating the impact of local anthropogenic emission, limited attention has been paid to the contribution from long-range transport. In this study, we apply simulations from six participating models supplied through the Task Force on Hemispheric Transport of Air Pollution phase 2 (HTAP2) exercise to investigate the long-range transport impact of Europe (EUR) and Russia–Belarus–Ukraine (RBU) on the surface air quality in eastern Asia(EAS), with special focus on their contributions during the haze episodes in China. The impact of 20 % anthropogenic emission perturbation from the source region is extrapolated by a factor of 5 to estimate the full impact.We find that the full impacts from EUR and RBU are 0.99 µg m -3 (3.1 %) and 1.32 µg m -3 (4.1 %) during haze episodes,while the annual averaged full impacts are only 0.35 µg m -3 (1.7 %) and 0.53 µg m -3 (2.6 %). By estimating the aerosol response within and above the planetary boundary layer (PBL), we find that long-range transport from EUR within the PBL contributes to 22–38 % of the total column density of aerosol response in EAS. Comparison with the HTAP phase 1 (HTAP1) assessment reveals that from 2000 to 2010, the long-range transport from Europe to eastern Asia has decreased significantly by a factor of 2–10 for surface aerosol mass concentration due to the simultaneous emission reduction in source regions and emission increase in the receptor region. We also find the long-range transport from the Europe and RBU regions increases the number of haze events in China by 0.15 % and 0.11 %, and the North China Plain and southeastern China has 1–3 extra haze days (<3 %). This study is the first investigation into the contribution of long-range transport to haze in China with multi-model experiments.

54 ENVIRONMENTAL SCIENCES↗

Low-Voltage Haze Tuning with Cellulose-Network Liquid Crystal Gels

Being key components of the building envelope, glazing products with tunable optical properties are in great demand because of their potential for boosting energy efficiency and privacy features while enabling the main function of allowing natural light indoors. However, windows and skylights with electric switching of haze and transparency are rare and often require high voltages or electric currents, as well as not fully meet the stringent technical requirements for glazing applications. Here, by introducing a predesigned gel material we describe an approach dubbed “Haze-Switch” that involves low-voltage tuning of the haze coefficient in a broad range of 2–90% while maintaining high visible-range optical transmittance. The approach is based on a nanocellulose fiber gel network infiltrated by a nematic liquid crystal, which can be switched between polydomain and monodomain spatial patterns of optical axis via a dielectric coupling between the nematic domains and the applied external electric field. By utilizing a nanocellulose network of nanofibers ~10 nm in diameter we achieve <10 V dielectric switching and <2% haze in the clear state, as needed for applications in window products. Finally, we characterize physical properties relevant to window and smart glass technologies, like the color rendering index, haze coefficient, and switching times, demonstrating that our material and envisaged products can meet the stringent requirements of the glass industry, including applications such as privacy windows, skylights, sunroofs, and daylighting.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Haze processing of atmospheric particles during wintertime in the Indo-Gangetic Plains

The impacts of haze on visibility, air quality, and climate are not well quantified due to a lack of understanding of the evolution of the mixing state and phase state of atmospheric particles during haze processing. The variability of the mixing state of atmospheric particles contributes significantly to uncertainties associated with the estimated aerosol radiative forcing. We collected particle samples in January 2018 from the highly polluted Indo-Gangetic plain during hazy conditions to study haze-processed particles. Single particle analysis using multi-modal micro-spectroscopy techniques revealed an abundance (40–70% by number) of potassium-rich sulfate particles from biomass-burning influenced smoke. Tilted view imaging showed that most of the organic particles that had inorganic potassium and sulfate inclusions were liquid-like while those without inclusions were more semi-solid. High-resolution mass spectrometry analysis revealed a significant presence of organosulfates and nitroxy-organosulfates in the morning samples (24%) compared to the afternoon samples (9%), despite higher relative humidity in the afternoon. Overall, our results highlight the significant contribution of both organic and inorganic sulfate to the total particulate sulfur budget during haze processing in winter, when anthropogenic emissions such as household burning, agricultural burning, and vehicular emissions are major contributors to particle mass.

Mathai, Susan [Pacific Northwest National Laborato↗

Black Carbon Amplifies Haze Over the North China Plain by Weakening the East Asian Winter Monsoon

Black carbon (BC) has previously been found to intensify haze in China by stabilizing the planetary boundary layer. With ocean, sea ice, and cloud feedbacks included in a global aerosol-climate model, we show here that BC emitted from the North China Plain can be transported to the oceans, which in turn changes cloud structure and land-sea thermal contrast. As a result, East Asian winter monsoon wind speeds decrease over the North China Plain. This decrease causes air stagnation that can further intensify haze. Our results suggest that in addition to the local BC-induced interactions between aerosol and the planetary boundary layer, BC can also amplify haze in the North China Plain by weakening East Asian winter monsoon through ocean, sea ice, and cloud feedbacks. It implies that reducing BC emissions could have significant indirect benefits for air quality in the North China Plain.

54 ENVIRONMENTAL SCIENCES↗

DENSECL: Haze Mitigation Using Dense Blocks and Contrastive Loss Regularization

Haze, which occurs as a result of the scattering of light in the atmosphere by small particles, diminishes the visibility of scene objects, inflicting important image applications such as object detection. To address the problem, this paper introduces a new physics-based end-to-end deep learning approach to haze mitigation in outdoor scenes, including those in airborne images. The proposed model named DenseCL is designed with dense blocks and adopts a contrastive loss function as an additional regularization. The model also maintains the cycle consistency by remapping the dehazed outputs into a hazy image using the physics-based light scattering function. DenseCL has been trained with publicly available outdoor images and demonstrates outstanding performance on outdoor, indoor, and remotely sensed nonhomogeneous haze satellite images.

Mitra, Somosmita↗

Haze Mitigation in High-Resolution Satellite Imagery using Enhanced Style-Transfer Neural Network and Normalization Across Multiple GPUs

Despite recent advances in deep learning approaches, haze mitigation in large satellite images is still a challenging problem. Due to amorphous nature of haze, object detection or image segmentation approaches are not applicable. Also it is practically infeasible to obtain ground truths for training. Bounded memory capacity of GPUs is another constraint that limits the size of image to be processed. In this paper, we propose a style transfer based neural network approach to mitigate haze in a large overhead imagery. The network is trained without paired ground truths; further, perception loss is added to restore vivid colors, enhance contrast and minimize artifacts. The paper also illustrates our use of multiple GPUs in a collective way to produce a single coherent clear image where each GPU dehazes different portions of a large hazy image.

Park, Byung↗

Aerosol hygroscopic growth, contributing factors, and impact on haze events in a severely polluted region in northern China

This study investigates the impact of the aerosol hygroscopic growth effect on haze events in Xingtai, a heavily polluted city in the central part of the North China Plain (NCP), using a large array of instruments measuring aerosol optical, physical, and chemical properties. Key instruments used and measurements made include the Raman lidar for atmospheric water vapor content and aerosol optical profiles, the PC-3016A GrayWolf six-channel handheld particle and mass meter for atmospheric total particulate matter (PM) that has diameters less than 1 and 2.5 µ m (PM 1 and PM 2.5 , respectively), the aerosol chemical speciation monitor (ACSM) for chemical components in PM 1 , and the hygroscopic tandem differential mobility analyzer (H-TDMA) for aerosol hygroscopicity. The changes in PM 1 and PM 2.5 agreed well with that of the water vapor content due to the aerosol hygroscopic growth effect. Two cases were selected to further analyze the effects of aerosol hygroscopic growth on haze events. The lidar-estimated hygroscopic enhancement factor for the aerosol backscattering coefficient during a relatively clean period (Case I) was lower than that during a pollution event (Case II) with similar relative humidity (RH) levels of 80 %–91 %. The Kasten model was used to fit the aerosol optical hygroscopic growth factor (GF) whose parameter b differed considerably between the two cases, i.e., 0.1000 (Case I) versus 0.9346 (Case II). The aerosol acidity value calculated from ACSM data for Case I (1.35) was less than that for Case II (1.50) due to different amounts of inorganics such as NH 4 NO 3 , NH 4 HSO 4 , and (NH 4 ) 2 SO 4 . Model results based on H-TDMA data showed that aerosol hygroscopic growth factors in each size category (40, 80, 110, 150, and 200 nm) at different RH levels (80 %–91 %) for Case I were lower than those for Case II. For similar ambient RH levels, the high content of nitrate facilitates the hygroscopic growth of aerosols, which may be a major factor contributing to heavy haze episodes in Xingtai.

Chen, Jun↗

Simulations of aerosol pH in China using WRF-Chem (v4.0): sensitivities of aerosol pH and its temporal variations during haze episodes

Aerosol pH is a fundamental property of aerosols in terms of atmospheric chemistry and its impact on air quality, climate, and health. Precise estimation of aerosol pH in chemical transport models (CTMs) is critical for aerosol modeling and thus influences policy development that partially relies on results from model simulations. We report the Weather Research and Forecasting Model coupled with Chemistry (WRF-Chem) simulated PM 2.5 pH over China during a period with heavy haze episodes in Beijing, and explore the sensitivity of the modeled aerosol pH to factors including emissions of nonvolatile cations (NVCs) and NH 3 , aerosol phase state assumption, and heterogeneous production of sulfate. We find that default WRF-Chem could predict spatial patterns of PM 2.5 pH over China similar to other CTMs, but with generally lower pH values, largely due to the underestimation of alkaline species (NVCs and NH 3 ) and the difference in thermodynamic treatments between different models. Increasing NH 3 emissions in the model would improve the modeled pH in comparison with offline thermodynamic model calculations of pH constrained by observations. In addition, we find that the aerosol phase state assumption and heterogeneous sulfate production are important in aerosol pH predictions for regions with low relative humidity (RH) and high anthropogenic SO 2 emissions, respectively. These factors should be better constrained in model simulations of aerosol pH in the future. Analysis of the modeled temporal trend of PM 2.5 pH in Beijing over a haze episode reveals a clear decrease in pH from 5.2 ± 0.9 in a clean period to 3.6 ± 0.5 in a heavily polluted period. The increased acidity under more polluted conditions is largely due to the formation and accumulation of secondary species including sulfuric acid and nitric acid, even though being modified by alkaline species (NVCs, NH 3 ). Our result suggests that NO 2 oxidation is unlikely to be important for heterogeneous sulfate production during the Beijing haze as the effective pH for NO 2 oxidation of S(IV) is at a higher pH of ~6.

54 ENVIRONMENTAL SCIENCES↗

Seesaw haze pollution in North China modulated by the sub-seasonal variability of atmospheric circulation

Utilizing a recent observational dataset of particulate matter with diameters less than 2.5 µ m (PM 2.5 ) in North China, this study reveals adistinct seesaw feature of abnormally high and low PM 2.5 concentrationsin the adjacent two months of December 2015 and January 2016, accompanied bydistinct meteorological modulations. The seesaw pattern is postulated to belinked to a super El Niño and the Arctic Oscillation (AO). During themature phase of El Niño in December 2015, the weakened East Asian wintermonsoon (EAWM) and the associated low-level southerly wind anomaly reducedplanetary boundary layer (PBL) height, favoring strong haze formation. Thiscirculation pattern was completely reversed in the following month, in partdue to a sudden phase change of the AO from positive to negative and thebeginning of a decay of the El Niño, which enhanced the southward shiftof the upper tropospheric jet from December to January relative toclimatology, leading to an enhanced EAWM and substantially lower hazeformation. This sub-seasonal change in circulation is also robustly found in1982–1983 and 1997–1998, implicative of a general physical mechanismdynamically linked to El Niño and the AO. Numerical experiments using theWeather Research and Forecasting (WRF) Community Multiscale Air Quality(CMAQ) model were used to test the modulation of the meteorologicalconditions on haze formation. With the same emission, simulations for threesuper El Niño periods (1983, 1997 and 2015) robustly show higherPM 2.5 concentrations under the mature phase of the super El Niño,but substantially lower PM 2.5 concentrations during the decay phase ofEl Niño (and the sudden AO phase change), further verifying themodulation effect of the sub-seasonal circulation anomaly on PM 2.5 concentrations in North China

54 ENVIRONMENTAL SCIENCES↗

Large Aerosol Particles Favor Haze Conditions Through Limitations on Water Budget and Activation Kinetics

Experiments in the Pi Convection‐Cloud Chamber conducted by systematically changing the diameter of injected dry aerosol particles while holding the temperature difference constant demonstrate that dry diameter strongly influences the onset of haze‐dominated conditions. Two factors contribute: the system becomes water‐limited, resulting in reduction of supersaturation by growing aerosol particles to the activation diameter; and the activation process becomes kinetically limited. Dry aerosol diameter exerts a strong influence on activation time, with a power‐law exponent of 9/2. Kinetically limited activation occurs when the ratio of the activation and droplet residence times is greater than unity. The findings demonstrate that a haze‐dominated state, where cloud formation is suppressed, can be achieved not only with weak supersaturation forcing and high aerosol concentration but also with large, hygroscopic aerosol particles. These results have implications for cloud formation in polluted environments, fog development near the ocean, and hygroscopic cloud seeding.

54 ENVIRONMENTAL SCIENCES↗