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- Johansson, Sofia M., 1983, et al.
(author)
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Experimental and Computational Study of Molecular Water Interactions with Condensed Nopinone Surfaces Under Atmospherically Relevant Conditions
- 2020
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In: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 124:18, s. 3652-3661
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Journal article (peer-reviewed)abstract
- Water and organics are omnipresent in the atmosphere, and their interactions influence the properties and lifetime of both aerosols and clouds. Nopinone is one of the major reaction products formed from beta-pinene oxidation, a compound emitted by coniferous trees, and it has been found in both gas and particle phases in the atmosphere. Here, we investigate the interactions between water molecules and nopinone surfaces by combining environmental molecular beam (EMB) experiments and molecular dynamics (MD) simulations. The EMB method enables detailed studies of the dynamics and kinetics of water interacting with solid nopinone at 170-240 K and graphite coated with a molecularly thin nopinone layer at 200-270 K. MD simulations that mimic the experimental conditions have been performed to add insights into the molecular-level processes. Water molecules impinging on nopinone surfaces are efficiently trapped (>= 97%), and only a minor fraction scatters inelastically while maintaining 35-65% of their incident kinetic energy (23.2 +/- 1.0 kJ mol(-1)). A large fraction (60-80%) of the trapped molecules desorbs rapidly, whereas a small fraction (20-40%) remains on the surface for more than 10 ms. The MD calculations confirm both rapid water desorption and the occurrence of strongly bound surface states. A comparison of the experimental and computational results suggests that the formation of surface-bound water clusters enhances water uptake on the investigated surfaces.
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| 3. |
- Johansson, Sofia M., 1983, et al.
(author)
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The Dynamics and Kinetics of Water Interactions with a Condensed Nopinone Surface.
- 2017
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In: The journal of physical chemistry. A. - : American Chemical Society (ACS). - 1520-5215 .- 1089-5639. ; 121:35
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Journal article (peer-reviewed)abstract
- Water and organic molecules are omnipresent in the environment, and their interactions are of central importance in many Earth system processes. Here we investigate molecular-level interactions between water and a nopinone surface using an environmental molecular beam (EMB) technique. Nopinone is a major reaction product formed during oxidation of β-pinene, a prominent compound emitted by coniferous trees, which has been found in both the gas and particle phases of atmospheric aerosol. The EMB method enables detailed studies of the dynamics and kinetics of D2O molecules interacting with a solid nopinone surface at 202 K. Hyperthermal collisions between water and nopinone result in efficient trapping of water molecules, with a small fraction that scatter inelastically after losing 60-80% of their incident kinetic energy. While the majority of the trapped molecules rapidly desorb with a time constant τ less than 10 μs, a substantial fraction (0.32 ± 0.09) form strong bonds with the nopinone surface and remain in the condensed phase for milliseconds or longer. The interactions between water and nopinone are compared to results for recently studied water-alcohol and water-acetic acid systems, which display similar collision dynamics but differ with respect to the kinetics of accommodated water. The results contribute to an emerging surface science-based view and molecular-level description of organic aerosols in the atmosphere.
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- Kong, Xiangrui, et al.
(author)
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Impact of SO2 and light on chemical morphology and hygroscopicity of natural salt aerosols
- 2024
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In: Atmospheric Environment. - 1352-2310 .- 1873-2844. ; 322
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Journal article (peer-reviewed)abstract
- The interactions between SO2 and natural salt aerosol particles represent complex and crucial dynamics within atmospheric processes and the broader climate system. This study investigated the SO2 uptake, hygroscopicity, morphology and mixing states of natural salt particles, which are generated from brines sampled from the Chaka salt lake located in the Qinghai-Tibet plateau. A comparison with atomized pure NaCl particles is included as reference. The results show that NaCl particles exhibit the lowest SO2 uptake, while Chaka salt particles demonstrate higher uptake due to their complex composition. The hygroscopicity of salt particles is influenced by several factors, including chemical complexity, SO2 exposure and light conditions. In comparison to pure NaCl, Chaka salt displays higher hygroscopicity, which is further enhanced in the presence of SO2. However, when exposed to light, mass growth is suppressed, suggesting the formation of species with lower hygroscopicity, such as Na2SO4. Analysis of particle morphology and mixing states reveals notable distinctions between NaCl crystals and Chaka salt particles, where the Chaka salt particles exhibit rounded shapes with a structure composed of cubic NaCl cores surrounded by sulfate materials as a coating. In addition, the chemical morphology analysis also reveals that the particles show morphological and spectral changes before and after the exposure to SO2, light and high RH. Therefore, this research highlights the intricate interactions between SO2 and natural salt aerosol particles in diverse environmental settings, underscoring their multifaceted impacts on atmospheric processes.
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| 6. |
- 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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| 7. |
- 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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| 10. |
- Priestley, Michael, et al.
(author)
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Volatility Measurements of Oxygenated Volatile Organics from Fresh and Aged Residential Wood Burning Emissions
- 2024
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In: ACS EARTH AND SPACE CHEMISTRY. - : American Chemical Society. - 2472-3452. ; 8:2, s. 159-173
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Journal article (peer-reviewed)abstract
- Residential wood combustion (RWC) is a dominant source of anthropogenic aerosol in urban areas. Complexities in aerosol chemical composition, semivolatile behavior, and secondary processing make estimating RWC impacts on climate and air quality challenging. A chemical ionization mass spectrometer with a filter inlet for gas and aerosols measured the gas-to-particle partitioning of organic compounds emitted from log wood and pellet burning stoves. Emissions were aged in an oxidation flow reactor to assess changes in the volatilities of the secondary aerosol. Effective saturation vapor concentrations (C*) of the measured species were derived using both the measured particle-to-gas concentration ratio (P- i/G( i)) and vapor pressure measurements (p(i)( 0)) calibrated using the maximum temperature during evaporation. These were used to derive new molecular formula (MF) parameterizations and were compared to selected previous parameterization. The fresh wood stove emissions were less volatile than those of the pellet stove (particle fractions of 0.96 vs 0.69), likely caused by poorer combustion conditions, producing a greater particle sink for organic vapors. After aging, the volatility of the emissions remained broadly similar, whereas all MF parameterizations showed increasing volatility. This was likely due to the measurement techniques capturing nonideal effects of partitioning that MF parameterizations cannot.
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