| 1. |
- Yue, Siyao, et al.
(author)
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Brown carbon from biomass burning imposes strong circum-Arctic warming
- 2022
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In: ONE EARTH. - : Elsevier BV. - 2590-3330 .- 2590-3322. ; 5:3, s. 293-304
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Journal article (peer-reviewed)abstract
- Rapid warming in the Arctic has a huge impact on the global environment. Atmospheric brown carbon (BrC) is one of the least understood and uncertain warming agents due to a scarcity of observations. Here, we performed direct observations of atmospheric BrC and quantified its light-absorbing properties during a 2 month circum-Arctic cruise in summer of 2017. Through observation-constrained modeling, we show that BrC, mainly originated from biomass burning in the mid-to high latitudes of the Northern Hemisphere (similar to 60%), can be a strong warming agent in the Arctic region, especially in the summer, with an average radiative forcing of-90 mW m(-2) (similar to 30% relative to black carbon). As climate change is projected to increase the frequency, intensity, and spread of wildfires, we expect BrC to play an increasing role in Arctic warming in the future.
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| 2. |
- Guo, Renjun, et al.
(author)
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Degradation mechanisms of perovskite solar cells under vacuum and one atmosphere of nitrogen
- 2021
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In: Nature Energy. - : Springer Nature. - 2058-7546. ; 6:10, s. 977-
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Journal article (peer-reviewed)abstract
- Extensive studies have focused on improving the operational stability of perovskite solar cells, but few have surveyed the fundamental degradation mechanisms. One aspect overlooked in earlier works is the effect of the atmosphere on device performance during operation. Here we investigate the degradation mechanisms of perovskite solar cells operated under vacuum and under a nitrogen atmosphere using synchrotron radiation-based operando grazing-incidence X-ray scattering methods. Unlike the observations described in previous reports, we find that light-induced phase segregation, lattice shrinkage and morphology deformation occur under vacuum. Under nitrogen, only lattice shrinkage appears during the operation of solar cells, resulting in better device stability. The different behaviour under nitrogen is attributed to a larger energy barrier for lattice distortion and phase segregation. Finally, we find that the migration of excessive PbI2 to the interface between the perovskite and the hole transport layer degrades the performance of devices under vacuum or under nitrogen. Understanding degradation mechanisms in perovskite solar cells is key to their development. Now, Guo et al. show a greater degradation of the perovskite structure and morphology for devices operated under vacuum than under nitrogen.
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| 3. |
- Li, Jun, et al.
(author)
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Hygroscopicity and Ice Nucleation Properties of Dust/Salt Mixtures Originating from the Source of East Asian Dust Storms
- 2022
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In: Frontiers in Environmental Science. - : Frontiers Media SA. - 2296-665X. ; 10
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Journal article (peer-reviewed)abstract
- Dust storms are common meteorological events that occur frequently in the late spring and early summer in arid and semi-arid areas. The resulting lofted dust and salt mixtures can impact atmospheric chemistry and climate systems through the many pathways represented by aerosol-cloud-climate interactions. In this study, dust/salt samples were collected from important sources of the East Asian dust storm, including the Badain Jaran Desert, the Tengger Desert and the Ulan Buh Desert in northwestern China. Ion chromatography (IC) measurements were performed to determine the concentrations of cations and anions. The ionic concentrations, pH and dissolvable fractions of sand samples show a positive correlation, indicating that the dissolved content is rich in alkaline ions. A positive matrix factorization (PMF) receptor model was employed to analyze the IC results, and from the PMF solutions non-obvious connections to local geography emerge. The results of hygroscopic experiments of sand samples which were measured by a vapor sorption analyzer indicate that the hygroscopicity may be related to the soluble content of samples, and the observed hygroscopic behavior can be well described by a thermodynamic model. The morphology of individual particles was chemically mapped by the synchrotron-based scanning transmission X-ray microscopy, and needle-shaped CaCO3 particles were observed to adhere to more irregular high K-containing particles. Moreover, a continuous flow diffusion chamber was used to investigate the ice nucleation abilities of typical salts, with both homogeneous freezing and deposition nucleation being observed. The results indicate that the salts primarily act as cloud condensation nuclei but can also act as ice nucleating particles at low temperatures.
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| 4. |
- Li, J., et al.
(author)
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Hygroscopicity of Fresh and Aged Salt Mixtures from Saline Lakes
- 2021
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In: Atmosphere. - : MDPI AG. - 2073-4433. ; 12:9
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Journal article (peer-reviewed)abstract
- The high hygroscopicity of salt aerosol particles makes the particles active in aerosol and cloud formations. Inland saline lakes are an important and dynamic source of salt aerosol. The salt particles can be mixed with mineral dust and transported over long distances. During transportation, these particles participate in atmospheric heterogeneous chemistry and further impact the climate and air quality on a global scale. Despite their importance and potential, relatively little research has been done on saline lake salt mixtures from atmospheric perspectives. In this study, we use experimental and model methods to evaluate the hygroscopic properties of saline lake brines, fresh salt aerosol particles, and aged salt aerosol particles. Both original samples and literature data are investigated. The original brine samples are collected from six salt lakes in Shanxi and Qinghai provinces in China. The ionic compositions of the brines are determined and the hygroscopicity measurements are performed on crystallized brines. The experimental results agree well with theoretical deliquescence relative humidity (DRH) values estimated by a thermodynamic model. The correlations between DRHs of different salt components and the correlations between DRHs and ionic concentrations are presented and discussed. Positive matrix factorization (PMF) analysis is performed on the ionic concentrations data and the hygroscopicity results, and the solutions are interpreted and discussed. The fresh and aged salt aerosol particles are analyzed in the same way as the brines, and the comparison shows that the aged salt aerosol particles completely alter their hygroscopic property, i.e., transferring from MgCl2- governed to NH4NO3- governed.
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| 5. |
- Deng, J., et al.
(author)
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Molecular markers for fungal spores and biogenic SOA over the Antarctic Peninsula: Field measurements and modeling results
- 2021
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In: Science of the Total Environment. - : Elsevier BV. - 0048-9697. ; 762:March
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Journal article (peer-reviewed)abstract
- Biogenic organic aerosols are important components of atmospheric organic aerosols and play vital roles in atmospheric chemistry, global climate, and biogeochemical cycles of carbon. However, studies on biogenic organic aerosols in the vast regions of the Southern Ocean and over the coastal waters of the Antarctic, especially Antarctic Peninsula, are still extremely limited. To understand the concentrations, molecular composition and seasonality of biogenic organic aerosols in Antarctica, atmospheric aerosols were collected at the Palmer Station on the west Antarctic Peninsula experiencing dramatic climate warming. Molecular marker compounds of fungal spores and secondary organic aerosols formed from the photooxidation of isoprene and monoterpene were analyzed using gas chromatography/mass spectrometry. Concentrations of sugar alcohols and biogenic SOA tracers both presented seasonal patterns with higher average concentrations in summer (90.7 and 122 pg m−3) than in winter (8.88 and 57.2 pg m−3). Sugar alcohols and biogenic SOA tracers were predominated by mannitol and isoprene oxidation products. Relative contributions of fungal-spore organic carbon (OC), isoprene-derived secondary OC (SOC) and monoterpene-derived SOC estimated with tracer-based methods were 26.2%, 55.6% and 18.2%, respectively. The observed seasonality of total biogenic SOA and some molecular species at the Antarctic Peninsula was further supported by the results from the global model CESM/IMPACT. Model results also suggest higher biogenic SOA in East Antarctica than that in West Antarctica, which is attributed to the influence of vertical atmospheric circulation. Our results of air-mass trajectory indicate the potential influence of marine emissions on the biogenic organic aerosols over the Antarctic Peninsula. © 2020 Elsevier B.V.
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| 6. |
- Fan, Jin, et al.
(author)
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Design of Ultra-Wideband Phased Array Feed for Radio Telescope
- 2020
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In: 2020 33rd General Assembly and Scientific Symposium of the International Union of Radio Science, URSI GASS 2020.
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Conference paper (peer-reviewed)abstract
- This paper presents an ultra-wideband Phased Array Feed (PAF) based on novel flat bend crossed dipole fed by 50Ohm coaxial line. The PAF is dual-polarized and made from all-metal to minimize Ohmic losses and simplify cryogenic integration. It is optimized for 1-2 GHz band and can be good PAF candidate for the Five hundred meter Aperture Spherical Telescope (FAST) and Qi Tai Telescope (QTT) as well as other radio telescopes.
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| 7. |
- Li, Linjie, et al.
(author)
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Gas-to-Particle Partitioning of Products from Ozonolysis of Δ3-Carene and the Effect of Temperature and Relative Humidity
- 2024
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In: JOURNAL OF PHYSICAL CHEMISTRY A. - 1089-5639 .- 1520-5215. ; 128:5, s. 918-928
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Journal article (peer-reviewed)abstract
- Formation of oxidized products from Delta(3)-carene (C10H16) ozonolysis and their gas-to-particle partitioning at three temperatures (0, 10, and 20 degrees C) under dry conditions (<2% RH) and also at 10 degrees C under humid (78% RH) conditions were studied using a time-of-flight chemical ionization mass spectrometer (ToF-CIMS) combined with a filter inlet for gases and aerosols (FIGAERO). The Delta(3)-carene ozonolysis products detected by the FIGAERO-ToF-CIMS were dominated by semivolatile organic compounds (SVOCs). The main effect of increasing temperature or RH on the product distribution was an increase in fragmentation of monomer compounds (from C-10 to C-7 compounds), potentially via alkoxy scission losing a C-3 group. The equilibrium partitioning coefficient estimated according to equilibrium partitioning theory shows that the measured SVOC products distribute more into the SOA phase as the temperature decreases from 20 to 10 and 0 degrees C and for most products as the RH increases from <2 to 78%. The temperature dependency of the saturation vapor pressure (above an assumed liquid state), derived from the partitioning method, also allows for a direct way to obtain enthalpy of vaporization for the detected species without accessibility of authentic standards of the pure substances. This method can provide physical properties, beneficial for, e.g., atmospheric modeling, of complex multifunctional oxidation products.
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| 8. |
- Ren, Hong, et al.
(author)
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Measurement report: Vertical distribution of biogenic and anthropogenic secondary organic aerosols in the urban boundary layer over Beijing during late summer
- 2021
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In: ATMOSPHERIC CHEMISTRY AND PHYSICS. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:17, s. 12949-12963
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Journal article (peer-reviewed)abstract
- Secondary organic aerosol (SOA) plays a significant role in atmospheric chemistry. However, little is known about the vertical profiles of SOA in the urban boundary layer (UBL). This knowledge gap constrains the SOA simulation in chemical transport models. Here, the aerosol samples were synchronously collected at 8, 120, and 260m based on a 325m meteorological tower in Beijing from 15 August to 10 September 2015. Strict emission controls were implemented during this period for the 2015 China Victory Day parade. Here, we observed that the total concentration of biogenic SOA tracers increased with height. The fraction of SOA from isoprene oxidation increased with height, whereas the fractions of SOA from monoterpenes and sesquiterpenes decreased, and 2,3-dihydroxy-4-oxopentanoic acid (DHOPA), a tracer of anthropogenic SOA from toluene oxidation, also increased with height. The complicated vertical profiles of SOA tracers highlighted the need to characterize SOA within the UBL. The mass concentration of estimated secondary organic carbon (SOC) ranged from 341 to 673 ngC m(-3). The increase in the estimated SOC fractions from isoprene and toluene with height was found to be more related to regional transport, whereas the decrease in the estimated SOC from monoterpenes and sesquiterpene with height was more subject to local emissions. Emission controls during the parade reduced SOC by 4 %-35 %, with toluene SOC decreasing more than the other SOC. This study demonstrates that vertical distributions of SOA within the UBL are complex, and the vertical profiles of SOA concentrations and sources should be considered in field and modeling studies in the future.
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| 9. |
- Salvador, Christian Mark, 1989, et al.
(author)
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Ambient nitro-aromatic compounds - biomass burning versus secondary formation in rural China
- 2021
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In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:3, s. 1389-1406
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Journal article (peer-reviewed)abstract
- Nitro-aromatic compounds (NACs) were measured hourly at a rural site in China during wintertime to monitor the changes due to local and regional impacts of biomass burning (BB). Concurrent and continuous measurements of the concentrations of 16 NACs in the gas and particle phases were performed with a time-of-flight chemical ionization mass spectrometer (CIMS) equipped with a Filter Inlet for Gases and AEROsols (FIGAERO) unit using iodide as the reagent ion. NACs accounted for <2 % of the mass concentration of organic matter (OM) and total particulate matter (PM), but the total particle mass concentrations of these compounds can reach as high as 1000 ng m(-3) (299 ng m(-3) avg), suggesting that they may contribute significantly to the radiative forcing effects of atmospheric particles. Levels of gas-phase NACs were highest during the daytime (15:00-16:00 local time, LT), with a smaller night-time peak around 20:00LT. Box-model simulations showed that this occurred because the rate of NAC production from gas-phase sources exceeded the rate of loss, which occurred mainly via the OH reaction and to a lesser degree via photolysis. Data gathered during extended periods with high contributions from primary BB sources (resulting in 40 %-60 % increases in NAC concentrations) were used to characterize individual NACs with respect to gas-particle partitioning and the contributions of regional secondary processes (i.e. photochemical smog). On days without extensive BB, secondary formation was the dominant source of NACs, and NAC levels correlated strongly with the ambient ozone concentration. Analyses of individual NACs in the regionally aged plumes sampled on these days allowed precursors such as phenol and catechol to be linked to their NAC derivatives (i.e. nitrophenol and nitrocatechol). Correlation analysis using the high time resolution data and box-model simulation results constrained the relationships between these compounds and demonstrated the contribution of secondary formation processes. Furthermore, 13 of 16 NACS were classified according to primary or secondary formation process. Primary emission was the dominant source (accounting for 60 %-70 % of the measured concentrations) of 5 of the 16 studied NACs, but secondary formation was also a significant source. Photochemical smog thus has important effects on brown carbon levels even during wintertime periods dominated by primary air pollution in rural China.
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| 10. |
- Thomsen, Ditte, et al.
(author)
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The effect of temperature and relative humidity on secondary organic aerosol formation from ozonolysis of Δ3-carene
- 2024
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In: Environmental Science: Atmospheres. - 2634-3606. ; 4:1, s. 88-103
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Journal article (peer-reviewed)abstract
- This study investigates the effects of temperature and relative humidity (RH) on the formation of secondary organic aerosol (SOA) from Δ3-carene, a prevalent monoterpene in boreal forests. Dark ozonolysis experiments of 10 ppb Δ3-carene were conducted in the Aarhus University Research on Aerosol (AURA) atmospheric simulation chamber at temperatures of 0, 10, and 20 °C. Under dry conditions (RH < 2%), the SOA formation in terms of both particle number and mass concentration shows minimal temperature dependence. This is in contrast to previous findings at higher initial concentrations and suggests an effect of VOC loading for Δ3-carene. Interestingly, the mass fraction of key oxidation products (cis-3-caric acid, cis-3-caronic acid) exhibit a temperature dependence suggesting continuous condensation at lower temperatures, while evaporation and further reactions over time become more favourable at higher temperatures. The oxygen-to-carbon ratios in the particle phase and the occurrence of highly oxygenated organic molecules (HOM) in the gas phase show modest increases with higher temperatures. Predictions from the Aerosol Dynamics and Gas- and Particle-Phase Chemistry Kinetic Multilayer Model (ADCHAM) agrees with the experimental results regarding both physical particle properties and aerosol composition considering the experimental uncertainties. At high RH (∼80%, 10 °C), a considerable increase in the particle nucleation rate and particle number concentration is observed compared to experiments under dry conditions. This is likely due to enhanced particle nucleation resulting from more stable cluster formation of water and inorganics at increased RH. However, RH does not affect the particle mass concentration.
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