Acidic air pollutants dissolve iron in aerosols and fertilize the ocean.

This study investigated the particle size‐ and age‐dependent mixing structures of individual particles in clean and polluted air. Aerosols were classified into eight components: sea salt, mineral dust, fly ash, metal, soot, sulfates, nitrates, and organic matter (OM). Based on our aerosol classification, a particle that consists of two or more aerosol components can be defined as an internally mixed particle. Otherwise, it is considered to be an externally mixed particle. Within the internally mixed particle class, we identified four heterogeneous mixing structures: core‐shell, dumbbell, OM coating, and dispersed OM, as well as one homogeneous‐like mixing structure. Homogeneous‐like mixing mainly occurred in fine particles (<1 µm), while the frequency of heterogeneously mixed particles increased with particle size. Our study demonstrated that particle mixing structures depend on particle size and location and evolve with time. OM‐coating and core‐shell structures are important indicators for particle aging in air as long as they are distant from specific emission sources. Long‐range transported particles tended to have core‐shell and OM‐coating structures. We found that secondary aerosol components (e.g., sulfates, nitrates, and organics) determined particle mixing structures, because their phases change following particle hydration and dehydration under different relative humidities. Once externally mixed particles are transformed into internally mixed particles, they cannot revert to their former state, except when semivolatile aerosol components are involved. Categorizing mixing structures of individual particles is essential for studying their optical and hygroscopic properties and for tracing the development of their physical or chemical properties over time.

Ammonium sulfate (AS) and ammonium nitrate (AN) are key components of urban fine particles. Both field and model studies showed that heterogeneous reactions of SO2, NO2, and NH3 on wet aerosols accelerated the haze formation in northern China. However, little is known on phase transitions of AS‐AN containing haze particles. Here hygroscopic properties of laboratory‐generated AS‐AN particles and individual particles collected during haze events in an urban site were investigated using an individual particle hygroscopicity system. AS‐AN particles showed a two‐stage deliquescence at mutual deliquescence relative humidity (MDRH) and full deliquescence relative humidity (DRH) and three physical states: solid before MDRH, solid‐aqueous between MDRH and DRH, and aqueous after DRH. During hydration, urban haze particles displayed a solid core and aqueous shell at RH = 60–80% and aqueous phase at RH > 80%. Most particles were in aqueous phase at RH > 50% during dehydration. Our results show that AS content in individual particles determines their DRH and AN content determines their MDRH. AN content increase can reduce MDRH, which indicates occurrence of aqueous shell at lower RH. The humidity‐dependent phase transitions of nitrate‐abundant urban particles are important to provide reactive surfaces of secondary aerosol formation in the polluted air.

In recent decades, air pollution has become an important environmental problem in the megacities of eastern China. How to control air pollution in megacities is still a challenging issue because of the complex pollutant sources, atmospheric chemistry, and meteorology. There is substantial uncertainty in accurately identifying the contributions of transport and local emissions to the air quality in megacities. The COVID-19 outbreak has prompted a nationwide public lockdown period and provides a valuable opportunity for understanding the sources and factors of air pollutants. The three-month period of continuous field observations for aerosol particles and gaseous pollutants, which extended from January 2020 to March 2020, covered urban, urban-industry, and suburban areas in the typical megacity of Hangzhou in the Yangtze River Delta in eastern China. In general, the concentrations of PM 2.5 – 10 , PM 2.5 , NO x , SO 2 , and CO reduced 58%, 47%, 83%, 11% and 30%, respectively, in the megacity during the COVID-Lock period. The reduction proportions of PM 2.5 and CO were generally higher in urban and urban-industry areas than those in suburban areas. NO x exhibited the greatest reduction (>80%) among all the air pollutants, and the reduction was similar in the urban, urban-industry, and suburban areas. O 3 increased 102%–125% during the COVID-Lock period. The daytime elevation of the planetary boundary layer height can reduce 30% of the PM 10 , PM 2.5 , NO x and CO concentrations on the ground in Hangzhou. During the long-range transport events, air pollutants on the regional scale likely contribute 40%–90% of the fine particles in the Hangzhou urban area. The findings highlight the future control and model forecasting of air pollutants in Hangzhou and similar megacities in eastern China.

Morphology, composition, and mixing state of individual particles emitted from crop residue, wood, and solid waste combustion in a residential stove were analyzed using transmission electron microscopy (TEM). Our study showed that particles from crop residue and apple wood combustion were mainly organic matter (OM) in smoldering phase, whereas soot-OM internally mixed with K in flaming phase. Wild grass combustion in flaming phase released some Cl-rich-OM/soot particles and cardboard combustion released OM and S-rich particles. Interestingly, particles from hardwood (pear wood and bamboo) and softwood (cypress and pine wood) combustion were mainly soot and OM in the flaming phase, respectively. The combustion of foam boxes, rubber tires, and plastic bottles/bags in the flaming phase released large amounts of soot internally mixed with a small amount of OM, whereas the combustion of printed circuit boards and copper-core cables emitted large amounts of OM with Br-rich inclusions. In addition, the printed circuit board combustion released toxic metals containing Pb, Zn, Sn, and Sb. The results are important to document properties of primary particles from combustion sources, which can be used to trace the sources of ambient particles and to know their potential impacts in human health and radiative forcing in the air.

We propose an approach to deal with the problem of freeform surface illumination design without assuming any symmetry based on the concept that this problem is similar to the problem of optimal mass transport. With this approach, the freeform design is converted into a nonlinear boundary problem for the elliptic Monge-Ampére equation. The theory and numerical method are given for solving this boundary problem. Experimental results show the feasibility of this approach in tackling this freeform design problem.

Surface plasmon resonance microscopy (SPRM) with single-direction illumination is a powerful platform for biomedical imaging because of its wide-field, label-free, and high-surface-sensitivity imaging capabilities. However, two disadvantages prevent wider use of SPRM. The first is its poor spatial resolution that can be as large as several micrometers. The second is that SPRM requires use of metal films as sample substrates; this introduces working wavelength limitations. In addition, cell culture growth on metal films is not as universally available as growth on dielectric substrates. Here we show that use of azimuthal rotation illumination allows SPRM spatial resolution to be enhanced by up to an order of magnitude. The metal film can also be replaced by a dielectric multilayer and then a different label-free surface-sensitive photonic microscopy is developed, which has more choices in terms of the working wavelength, polarization, and imaging section, and will bring opportunities for applications in biology.

Abstract. Many studies have focused on the physicochemical properties of aerosol particles in unusually severe haze episodes in North China instead of the more frequent and less severe hazes. Consistent with this lack of attention, the morphology and mixing state of organic matter (OM) particles in the frequent light and moderate (L &amp; M) hazes in winter in the North China Plain (NCP) have not been examined, even though OM dominates these fine particles. In the present work, morphology, mixing state, and size of organic aerosols in the L &amp; M hazes were systematically characterized using transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy, atomic force microscopy, and nanoscale secondary ion mass spectrometer, with the comparisons among an urban site (Jinan, S1), a mountain site (Mt. Tai, S2), and a background island site (Changdao, S3) in the same hazes. Based on their morphologies, the OM particles were divided into six different types: spherical (type 1), near-spherical (type 2), irregular (type 3), domelike (type 4), dispersed-OM (type 5), and OM-coating (type 6). In the three sampling sites, types 1–3 of OM particles were most abundant in the L &amp; M hazes and most of them were internally mixed with non-OM particles. The abundant near-spherical OM particles with higher sphericity and lower aspect ratio indicate that these primary OM particles formed in the cooling process after polluted plumes were emitted from coal combustion and biomass burning. Based on the Si-O-C ratio in OM particles, we estimated that 71 % of type 1–3 OM particles were associated with coal combustion. Our result suggests that coal combustion in residential stoves was a widespread source from urban to rural areas in NCP. Average OM thickness which correlates with the age of the air masses in type 6 particles only slightly increased from S1 to S2 to S3, suggesting that the L &amp; M hazes were usually dry (relative humidity < 60 %) with weak photochemistry and heterogeneous reactions between particles and gases. We conclude that the direct emissions from these coal stoves without any pollution controls in rural areas and in urban outskirts contribute large amounts of primary OM particles to the regional L &amp; M hazes in North China.