Highly branched bolapolyphilic liquid crystals with a cubic A15 network at the triangle-square transition.

Rod-like bolapolyphiles with highly branched carbosilane-based side-chains self-assemble into several honeycomb structures if the oligo(p-phenylene ethynylene) core is polyfluorinated, whereas for the non-fluorinated series an A15 type cubic network of rod-bundles was observed instead, suggesting a brand new pathway for the transition between triangular and square honeycomb phases.

Parameterization of the ambient aerosol refractive index with source appointed chemical compositions.

The refractive index of ambient aerosols is widely used in the climate model and remote sensing. Traditionally, the real part of the refractive index (RRI) of the ambient aerosol is calculated from the measured mass fraction of the main inorganic components with known refractive index, without full resolving the effects of variation in the RRI of organic components, which always contribute more than 50 % of the total aerosol mass. For the first time, the ambient aerosol RRI and the aerosol chemical components were measured concurrently at a suburban site Changping, in Beijing, China. Measurements results show that the ambient aerosol ranges between 1.57 and 1.71 with a mean value of 1.66. The mean mass fractions of organic aerosol (OA), nitrate, sulfate, ammonium, and chloride to total non-refractory aerosol loading are 43.1 %, 21.9 %, 21.6 %, 13.1 %, and 0.3 % respectively. Source appointment analysis of the organic aerosol show that the fossil fuel-related OA, cooking OA, biomass burning OA, less oxidized oxygenated OA and more oxidized OOA contributes 18.0 %, 11.2 %, 4.1 %, 39.9 %, 26.7 % to the total aerosol. A new parameterization scheme of the ambient aerosol RRI, which considers the source appointed OA, is proposed based on the concurrent measurements of RRI and chemical composition. The measured and parameterized RRI shows good consistency with a correlation coefficient of 0.79 and slope of 0.98. Our measurement results reveal that a significant deviation of the calculated RRI exists without considering the variation of the RRI of the aerosol organic component. The parametrization scheme is adopted and applicable in aerosol model for bettering estimating the corresponding optical and radiative effects.

Understanding and Manipulating Helical Nanofilaments in Binary Systems with Achiral Dopants.

Here, we report the relationship between helical pitch of the helical nanofilament (HNF) phase formed by bent-core molecule NOBOW and the concentration of achiral dopants 5CB and octane, using linearly polarized resonant soft X-ray scattering (RSoXS). Utilizing theory-based simulation, which fits well with the experiments, the molecular helices in the filament were probed and the superstructure of helical 5CB directed by groove of HNFs was observed. Quantitative pitch determination with RSoXS reveals that helical pitch variation is related to 5CB concentration with no temperature dependence. Doping rodlike immiscible 5CB led to a pitch shortening of up to 30%, which was attributed to a change in interfacial tension. By shedding light not only on phase behavior of binary systems but also enabling control over pitch length, our work may benefit various applications of HNF-containing binary systems, including optical rotation devices, circularly polarized light emitters, and chirality transfer agents.

Current challenges of improving visibility due to increasing nitrate fraction in PM2.5 during the haze days in Beijing, China.

The annual mean PM2.5 mass concentration has decreased because of the stringent emission controls implemented in Beijing, China in recent years, whereas the nitrate NO3- mass fraction in PM2.5 increases gradually. Low-visibility events occur frequently even though PM2.5 pollution has been mitigated significantly, with the daily mean PM2.5 mass concentration mostly less than 75 µg/m3. In this study, the non-linear relationship was analyzed between atmospheric visibility and PM2.5 based on chemical composition from a two-year field observation. Our results showed that NO3- became the main constituent of PM2.5, especially during the haze pollution episodes. A localized parameterization scheme was proposed between the atmospheric extinction coefficient (σext) and major chemical constituents of PM2.5 by multiple linear regression (MLR). The contribution of NO3- to σext increased with increasing air pollution, and NO3- became the most important contributor for PM2.5 above 75 µg/m3. The visibility decreased with increasing NO3- mass fraction for the same PM2.5 mass concentration when PM2.5 was above 20 µg/m3. The hygroscopicity of PM2.5 increased with increasing mass fraction of hygroscopic NO3-. These results stressed the importance of reducing particulate NO3- and its precursors (for instance, NH3) through effective emission control measures as well as the tightening of PM2.5 standards to further improve air quality and visibility in Beijing.

Asymmetric Incorporation of Silver Nanoparticles in Polymeric Assemblies by Coassembly of Tadpole-Like Nanoparticles and Amphiphilic Block Copolymers.

A general approach to asymmetrically localize nanoparticles (NPs) in larger polymeric nanostructures is demonstrated by coassembly of tadpole-like silver NPs (AgNPs) and amphiphilic block copolymers (BCPs). The tadpole-like AgNPs are prepared by template synthesis using a tailor-made A(BC)20 star polymer, namely poly(ethylene glycol)[poly(acrylic acid)-block-polystyrene]20 [PEG(PAA-b-PS)20 ], as template resulting in AgNPs decorated with twenty short PS chains and one long PEG chain, named Ag@PEG(PS)20 . The asymmetric distribution of these AgNPs in various polymeric nanostructures, e.g., spherical micelles, cylindrical micelles, vesicles, and sponge phase, is achieved via coassembly of the as-prepared Ag@PEG(PS)20 and PEG-b-PS in solution driven by the anisotropic nature of the Ag@PEG(PS)20 . This report not only provides a new strategy for the fabrication of tadpole-like NPs but also offers opportunity for off-center distributing NPs in hybrid assemblies, which may find applications in, e.g., sensing, catalysis, and diagnostics.

The particle phase state during the biomass burning events.

The phase state of biomass burning aerosols (BBA) remains largely unclear, impeding our understanding of their effects on air quality, climate and human health, due to its profound roles in mass transfer between gaseous and particulate phase. In this study, the phase state of BBA was investigated by measuring the particle rebound fraction ƒ combining field observations and laboratory experiments. We found that both ambient and laboratory-generated BBA had unexpectedly lower rebound fraction ƒ (<0.6) under the dry conditions (RH = 20-50%), indicating that BBA were in non-solid state at such low RH. This was obviously different from the secondary organic aerosols (SOA) derived from the oxidation of both anthropogenic and biogenic volatile organic compounds, typically with a rebound fraction ƒ larger than 0.8 at RH below 50%. Therefore, we proposed that the diffusion coefficient of gaseous molecular in the bulk of BBA might be much higher than SOA under the dry conditions.

Larger than expected variation range in the real part of the refractive index for ambient aerosols in China.

The real part of the refractive index (RRI) of ambient aerosol, which is widely used in remote sensing and atmospheric models, is one of the key factors determining its particles' optical properties. The characteristics of ambient aerosol RRI in China have not yet been well studied owing to a lack of observations. For the first time, the properties of aerosol RRI were studied based on field measurements in China at four sites with different atmospheres. The results revealed that the measured ambient aerosol RRI varied significantly between 1.36 and 1.78, increasing with the mass ratio of organic components. The scattering coefficient and direct radiative effects of the aerosols were estimated to increase by factors of 2 and 3, respectively, when RRI increased from 1.36 to 1.78. Our results indicate that variation in ambient aerosol RRI should be considered in aerosol and climate models to achieve an accurate estimation of aerosol's radiative impacts.

Explosive Secondary Aerosol Formation during Severe Haze in the North China Plain.

Severe haze events with exceedingly high-levels of fine aerosols occur frequently over the past decades in the North China Plain (NCP), exerting profound impacts on human health, weather, and climate. The development of effective mitigation policies requires a comprehensive understanding of the haze formation mechanisms, including identification and quantification of the sources, formation, and transformation of the aerosol species. Haze evolution in this region exhibits distinct physical and chemical characteristics from clean to polluted periods, as evident from increasing stagnation and relative humidity, but decreasing solar radiation as well as explosive secondary aerosol formation. The latter is attributed to highly elevated concentrations of aerosol precursor gases and is reflected by rapid increases in the particle number and mass concentrations, both corresponding to nonequilibrium chemical processes. Considerable new knowledge has been acquired to understand the processes regulating haze formation, particularly in light of the progress in elucidating the aerosol formation mechanisms. This review synthesizes recent advances in understanding secondary aerosol formation, by highlighting several critical chemical/physical processes, that is, new particle formation and aerosol growth driven by photochemistry and aqueous chemistry as well as the interaction between aerosols and atmospheric stability. Current challenges and future research priorities are also discussed.

A preliminary investigation of COVID-19 transmission in the United States by incorporating social media sentiments.

COVID-19 has now become a global pandemic. During the widespread of COVID-19, Twitter, as an online social media platform, has been a preferred channel for interaction and communication. As a result, it provides huge amount of information from which latent signals such as sentiments can be mined for a better understanding of COVID-19 transmission patterns. As a preliminary attempt, we reveal a strongly positive zero-order correlation between sentiments of tweets and COVID-19 confirmed cases in U.S. Considering the unique hierarchical structure of the U.S. government, state governments exert their own power to issue public health policies. Indeed, there are different patterns of correlations between sentiments and COVID-19 confirmed cases, affirming that country-level characteristics suppress that of state-level. Diving deeper into the textual content of COVID-19 related tweets, there manifests a diverse set of topics which in turn lead to dispersed sentiments. Our preliminary investigation paves the way for a finer-grained analysis of the COVID-19 transmission and social media activities by considering varying situations across states and topics.

Intensity-noise suppression in 1950-nm single-frequency fiber laser by bidirectional amplifier configuration.

In this Letter, a bidirectional amplifier configuration suppressing the relative intensity noise in a 1950-nm linearly polarized single-frequency fiber laser (SFFL) is proposed. The scheme to amplify the signal in a nonlinear saturated amplification regime with low gain distribution for suppressing the RIN is theoretically analyzed. By optimizing the input power level and reflectivity of the bidirectional power-amplifier, the RIN is decreased maximally by >24dB within the frequency range of 200 kHz. A stable output power of over 5.16 W with a polarization extinction ratio of 21.2 dB is obtained. Additionally, the amplified signal maintains a linewidth of 7.1 kHz nearly identical with that of the seed, both with a signal-to-noise ratio of more than 60 dB. This all-optical technique on noise suppression applied to the fiber amplifier paves the way to realize low-noise SFFL with power improvement.

Noise-sideband-free and narrow-linewidth photonic microwave generation based on anoptical heterodyne technique of low-noise fiber lasers.

Noise-sideband-free and narrow-linewidth photonic microwave generation based on an optical heterodyne technique is demonstrated experimentally. By beating a self-injection-locking low-noise single-frequency fiber laser and a Brillouin fiber laser, a 9.4 GHz microwave is produced, and its noise sidebands are completely suppressed. Additionally, the signal-to-noise ratio of the microwave signal is improved by 15 dB from 40 to 55 dB, and the linewidth is compressed from 1.6 to 0.53 kHz. The high-performance photonic microwave based on low-noise fiber lasers is a promising candidate in further applications such as wireless network, lidar, and satellite communication.

55 W kilohertz-linewidth core- and in-band-pumped linearly polarized single-frequency fiber laser at 1950 nm.

Based on core- and in-band-pumped polarization-maintaining ${{\rm Tm}^{3 + }}$Tm3+-doped single-cladding fiber (PM-TSF, the core diameter is 9 µm) by a 1610 nm fiber laser and a distributed Bragg reflector seed laser, a linearly polarized single-frequency fiber laser (LP-SFFL) at 1950 nm with an output power of 55.3 W and a laser linewidth of 6.95 kHz is demonstrated. The output beam qualities of ${M}_x^2$Mx2 and ${ M}_y^2$My2 are measured to be 1.01 and 1.03, respectively. The slope efficiency with respect to the launched pump power is 71.0%, in comparison with a theoretical quantum efficiency of 82.6%. A polarization-extinction ratio of 19 dB and an optical signal-to-noise ratio of 58 dB are obtained from the 1950 nm LP-SFFL. To the best of our knowledge, to date, this is the highest power of 2.0 µm SFFL output directly from a strict single-mode active fiber. Our experiment offers a promising solution to the current limitations of the high-performance fiber lasers at 2.0 µm, which is particularly essential for coherent detection.

Luminescent Metallacycle-Cored Liquid Crystals Induced by Metal Coordination.

Two rhomboidal metallacycles based on metal-coordination-driven self-assembly are presented. Because metal-coordination interactions restrict the rotation of phenyl groups on tetraphenylethene units, these metallacycles were emissive both in solution and in solid state, and their aggregation-induced emission properties were well-retained. Moreover, the rhomboidal metallacyclic structures offer a platform for intermolecular packing beneficial for the formation of liquid crystalline phases. Therefore, although neither of building blocks shows mesogenic properties, both thermotropic and lyotropic (in DMF) mesophases were observed in one of metallacycles, indicating that mesophases could be induced by metal-coordination interactions. This study not only reveals the mechanism for the formation of cavity-cored liquid crystals, but also provides a convenient approach to preparing supramolecular luminescent liquid crystals, which will serve as good candidates for chemo sensors and liquid crystal displays.

Enhancement in Particulate Organic Nitrogen and Light Absorption of Humic-Like Substances over Tibetan Plateau Due to Long-Range Transported Biomass Burning Emissions.

To elucidate the influence of long-range transported biomass burning organic aerosols (BBOA) on the Tibetan Plateau, the molecular compositions and light absorption of HUmic-Like Substances (HULIS), major fractions of brown carbon, were characterized during the premonsoon season. Under the significant influence of biomass burning, HULIS concentrations increased to as high as 26 times of the background levels, accounting for 54% of water-soluble organic carbon (WSOC) and 50% of organic carbon (OC). The light absorption of HULIS also enhanced up to 42 times of the background levels, contributing 61% of the WSOC absorption and 50% of OC absorption. Meanwhile, elevated nitrogen-containing compounds (NOCs) among HULIS were observed. The NOCs from fresh and aged BBOA were unambiguously identified on the molecular level, through comparing with the molecular compositions of NOCs from lab-controlled and field burning experiments. N-Heterocyclic bases represent major fractions in the reduced nitrogen compounds from fresh BBOA, and nitroaromatic compounds are important groups among the oxidized nitrogen compounds from aged BBOA. The nitrogen-containing compounds, including nitroaromatics and N-heterocyclic compounds, were also important chromophores, which contributed to the enhanced light absorption of extracted HULIS during biomass burning-influenced periods.

New insight into PM2.5 pollution patterns in Beijing based on one-year measurement of chemical compositions.

In recent years, air pollution has become a major concern in China, especially in the capital city of Beijing. Haze events occur in Beijing over all four seasons, exhibiting distinct characteristics. In this study, the typical evolution patterns of atmospheric particulate matter with a diameter of less than 2.5µm (PM2.5) in each season were illustrated by episode-based analysis. In addition, a novel method was developed to elucidate the driving species of pollution, which is the largest contributor to the incremental PM2.5 (ΔPM2.5), not PM2.5. This method revealed a temporal variation of the driving species throughout the year: nitrate-driven spring, sulfate-driven summer, nitrate-driven early fall, and organic matters (OM)-driven late fall and winter. These results suggested that primary organic particles or volatile organic compounds emissions were dominant in the heating season due to residential heating, while NOx and SO2 emissions dominated in the other seasons. Besides, nitrate formation seemed more significant than sulfate formation during severe pollution episodes. It was also found that the pollution formation mechanism in the winter showed some unique features in comparison with the other seasons: aqueous reactions were more important in the winter, while multiple pathways coexisted in the other seasons. Furthermore, this study confirmed that the PM2.5 in Beijing was moderately acidic despite a fully neutralized system. In addition, the acidity variation during pollution episodes displayed different patterns between seasons and was driven by both the variation of aerosol water and chemical compositions. These results provide a new perspective to understand the characteristics and mechanisms of aerosol pollution in Beijing. However, more accurate measurements are necessary for effective air pollution control that depends on the seasonal variation of fine particle formation in Beijing and the surrounding areas.

Temporal and spatial distribution of PM2.5 chemical composition in a coastal city of Southeast China.

Rapid economic development and urbanization in China has been concentrated in coastal cities, resulting in haze and photochemical smog issues, especially in the densely-populated Yangtze River Delta. In this study, we explore particulate matter (specifically PM2.5) pollution in a city in Zhejiang Province (Ningbo), chosen to represent a typical, densely-populated urban city with residential and industrial sections. PM2.5 samples were collected at five sites in four seasons from Dec. 2012 to Nov. 2013. The annual average PM2.5 mass concentration was 53.2±30.4µg/m3, with the highest concentration in winter and lowest in summer. Among the five sites, PM2.5 concentration was highest in an urban residential site and lowest in a suburban site, due to effects of urbanization and the anthropogenic influences. The chemical components of PM2.5 show significant seasonal variation. In addition, secondary transformation was high in Ningbo, with the highest proportion of secondary components found at a suburban site and the lowest at the industrial sites. Ningbo is controlled by five major air masses originating from inland China, from the Bohai Sea, offshore from the southeast, the Yellow Sea, and off the east coast of Korea. The relative contributions of these air masses differ, by season, with the Bohai Sea air mass dominating in winter and spring, the maritime southeast air mass in summer, and the Yellow Sea and coastal Korean air masses dominating in autumn. The continental air mass is associated with a high PM2.5 concentration, indicating that it is primarily transports primary emissions. In contrast, the concentration ratios among secondary formed pollutants were higher in the maritime air masses, which suggests that sea breezes control temporal and spatial variations of air pollution over coastal cities.