Survival probability of new atmospheric particles : closure between theory and measurements from 1.4 to 100 nm

The survival probability of freshly nucleated particles governs the influences of new particle formation (NPF) on atmospheric environments and the climate. It characterizes the probability of a particle avoiding being scavenged by the coagulation with pre-existing particles and other scavenging processes before the particle successfully grows up to a certain diameter. Despite its importance, measuring the survival probability has been challenging, which limits the knowledge of particle survival in the atmosphere and results in large uncertainties in predicting the influences of NPF. Here we report the proper methods to retrieve particle survival probability using the measured aerosol size distributions. Using diverse aerosol size distributions from urban Beijing, the Finnish boreal forest, a chamber experiment, and aerosol kinetic simulations, we demonstrate that each method is valid for a different type of aerosol size distribution, whereas misapplying the conventional methods to banana-type NPF events may underestimate the survival probability. Using these methods, we investigate the consistency between the measured survival probability of new particles and the theoretical survival probability against coagulation scavenging predicted using the measured growth rate and coagulation sink. With case-by-case and time- and size-resolved analysis of long-term measurement data from urban Beijing, we find that although both the measured and theoretical survival probabilities are sensitive to uncertainties and variations, they are, on average, consistent with each other for new particles growing from 1.4 (the cluster size) to 100 nm.Peer reviewe

The contribution of new particle formation and subsequent growth to haze formation

We investigated the contribution of atmospheric new particle formation (NPF) and subsequent growth of the newly formed particles, characterized by high concentrations of fine particulate matter (PM2.5). In addition to having adverse effects on visibility and human health, these haze particles may act as cloud condensation nuclei, having potentially large influences on clouds and precipitation. Using atmospheric observations performed in 2019 in Beijing, a polluted megacity in China, we showed that the variability of growth rates (GR) of particles originating from NPF depend only weakly on low-volatile vapor - highly oxidated organic molecules (HOMs) and sulphuric acid - concentrations and have no apparent connection with the strength of NPF or the level of background pollution. We then constrained aerosol dynamic model simulations with these observations. We showed that under conditions typical for the Beijing atmosphere, NPF is capable of contributing with more than 100 mu g m(-3) to the PM2.5 mass concentration and simultaneously >10(3) cm(-3) to the haze particle (diameter > 100 nm) number concentration. Our simulations reveal that the PM2.5 mass concentration originating from NPF, strength of NPF, particle growth rate and pre-existing background particle population are all connected with each other. Concerning the PM pollution control, our results indicate that reducing primary particle emissions might not result in an effective enough decrease in total PM2.5 mass concentrations until a reduction in emissions of precursor compounds for NPF and subsequent particle growth is imposed.Peer reviewe

Thermal Emission from the Hot Jupiter WASP-103b in JJ and KsK_{\rm s} Bands

Hot Jupiters, particularly those with temperature higher than 2000\,K are the best sample of planets that allow in-depth characterization of their atmospheres. We present here a thermal emission study of the ultra hot Jupiter WASP\mbox{-}103\,b observed in two secondary eclipses with CFHT/WIRCam in $J$ and $K_{\rm s}$ bands. By means of high precision differential photometry, we determine eclipse depths in $J$ and $K_{\rm s}$ to an accuracy of 220 and 270\,ppm, which are combined with the published HST/WFC3 and Spitzer data to retrieve a joint constraints on the properties of WASP-103\,b dayside atmosphere. We find that the atmosphere is best fit with a thermal inversion layer included. The equilibrium chemistry retrieval indicates an enhanced C/O (1.35$^{+0.14}_{-0.17}$) and a super metallicity with [Fe/H]$=2.19^{+0.51}_{-0.63}$ composition. Given the near-solar metallicity of WASP-103 of [Fe/H]=0.06, this planet seems to be $\sim$100 more abundant than its host star. The free chemistry retrieval analysis yields a large abundance of FeH, H$^{-}$, CO$_2$ and CH$_4$. Additional data of better accuracy from future observations of JWST should provide better constraint of the atmospheric properties of WASP-103b

Precursor apportionment of atmospheric oxygenated organic molecules using a machine learning method

Publisher Copyright: © 2023 The Author(s). Published by the Royal Society of Chemistry.Gas-phase oxygenated organic molecules (OOMs) can contribute significantly to both atmospheric new particle growth and secondary organic aerosol formation. Precursor apportionment of atmospheric OOMs connects them with volatile organic compounds (VOCs). Since atmospheric OOMs are often highly functionalized products of multistep reactions, it is challenging to reveal the complete mapping relationships between OOMs and their precursors. In this study, we demonstrate that the machine learning method is useful in attributing atmospheric OOMs to their precursors using several chemical indicators, such as O/C ratio and H/C ratio. The model is trained and tested using data acquired in controlled laboratory experiments, covering the oxidation products of four main types of VOCs (isoprene, monoterpenes, aliphatics, and aromatics). Then, the model is used for analyzing atmospheric OOMs measured in both urban Beijing and a boreal forest environment in southern Finland. The results suggest that atmospheric OOMs in these two environments can be reasonably assigned to their precursors. Beijing is an anthropogenic VOC dominated environment with ~64% aromatic and aliphatic OOMs, and the other boreal forested area has ~76% monoterpene OOMs. This pilot study shows that machine learning can be a promising tool in atmospheric chemistry for connecting the dots.Peer reviewe

Contribution of Atmospheric Oxygenated Organic Compounds to Particle Growth in an Urban Environment

Gas-phase oxygenated organic molecules (OOMs) can contribute substantially to the growth of newly formed particles. However, the characteristics of OOMs and their contributions to particle growth rate are not well understood in urban areas, which have complex anthropogenic emissions and atmospheric conditions. We performed long-term measurement of gas-phase OOMs in urban Beijing during 2018-2019 using nitrate-based chemical ionization mass spectrometry. OOM concentrations showed clear seasonal variations, with the highest in the summer and the lowest in the winter. Correspondingly, calculated particle growth rates due to OOM condensation were highest in summer, followed by spring, autumn, and winter. One prominent feature of OOMs in this urban environment was a high fraction (similar to 75%) of nitrogen-containing OOMs. These nitrogen-containing OOMs contributed only 50-60% of the total growth rate led by OOM condensation, owing to their slightly higher volatility than non-nitrate OOMs. By comparing the calculated condensation growth rates and the observed particle growth rates, we showed that sulfuric acid and its clusters are the main contributors to the growth of sub-3 nm particles, with OOMs significantly promoting the growth of 3-25 nm particles. In wintertime Beijing, however, there are missing contributors to the growth of particles above 3 nm, which remain to be further investigated.Peer reviewe

Properties and Asteroseismological analysis of a new ZZ ceti discovered by TMTS

Tsinghua university-Ma Huateng Telescope for Survey (TMTS) aims to discover rapidly evolving transients by monitoring the northern sky. The TMTS catalog is cross-matched with the white dwarf (WD) catalog of Gaia EDR3, and light curves of more than a thousand WD candidates are obtained so far. Among them, the WD TMTS J23450729+5813146 (hereafter J2345) is one interesting common source. Based on the light curves from the TMTS and follow-up photometric observations, periods of 967.113 s, 973.734 s, 881.525 s, 843.458 s, 806.916 s and 678.273 s are identified. In addition, the TESS observations suggest a 3.39 h period but this can be attributed to the rotation of a comoving M dwarf located within 3". The spectroscopic observation indicates that this WD is DA type with Teff = 11778+/-617K,log g = 8.38+/-0.31,mass=0.84+/-0.20Msun and age=0.704+/-0.377 Gyrs. Asteroseismological analysis reveals a global best-fit solution of Teff =12110+/-10K and mass=0.760+/-0.005Msun,consistent with the spectral fitting results, and Oxygen and Carbon abundances in the core center are 0.73 and 0.27, respectively. The distance derived from the intrinsic luminosity given by asteroseismology is 93 parsec, which is in agreement with the distance of 98 parsec from Gaia DR3. Additionally, kinematic study shows that this WD is likely a thick disk star. The mass of its zero-age main-sequence mass is estimated to be 3.08 Msun and has a main-sequence plus cooling age of roughly 900 Myrs.Comment: 10 pages, 10 figures, accepted for publication in MNRA

Seasonal variation in oxygenated organic molecules in urban Beijing and their contribution to secondary organic aerosol

Oxygenated organic molecules (OOMs) are crucial for atmospheric new particle formation and secondary organic aerosol (SOA) growth. Therefore, understanding their chemical composition, temporal behavior, and sources is of great importance. Previous studies on OOMs mainly focus on environments where biogenic sources are predominant, yet studies on sites with dominant anthropogenic emissions, such as megacities, have been lacking. Here, we conducted long-term measurements of OOMs, covering four seasons of the year 2019, in urban Beijing. The OOM concentration was found to be the highest in summer (1.6 x 10(8) cm(-3)), followed by autumn (7.9 x 10(7) cm(-3)), spring (5.7 x 10(7) cm(-3)) and winter (2.3 x 10(7) cm(-3)), suggesting that enhanced photo-oxidation together with the rise in temperature promote the formation of OOMs. Most OOMs contained 5 to 10 carbon atoms and 3 to 7 effective oxygen atoms (nO(eff) = nO - 2 x nN). The average nO(eff )increased with increasing atmospheric photo-oxidation capacity, which was the highest in summer and the lowest in winter and autumn. By performing a newly developed workflow, OOMs were classified into the following four types: aromatic OOMs, aliphatic OOMs, isoprene OOMs, and monoterpene OOMs. Among them, aromatic OOMs (29 %-41 %) and aliphatic OOMs (26 %-41 %) were the main contributors in all seasons, indicating that OOMs in Beijing were dominated by anthropogenic sources. The contribution of isoprene OOMs increased significantly in summer (33 %), which is much higher than those in the other three seasons (8 %-10 %). Concentrations of isoprene (0.2-5.3 x 10(7) cm(-3)) and monoterpene (1.1-8.4 x 10(6) cm(-3)) OOMs in Beijing were lower than those reported at other sites, and they possessed lower oxygen and higher nitrogen contents due to high NO, levels (9.5-38.3 ppbv - parts per billion by volume) in Beijing. With regard to the nitrogen content of the two anthropogenic OOMs, aromatic OOMs were mainly composed of CHO and CHON species, while aliphatic OOMs were dominated by CHON and CHON2 ones. Such prominent differences suggest varying formation pathways between these two OOMs. By combining the measurements and an aerosol dynamic model, we estimated that the SOA growth rate through OOM condensation could reach 0.64, 0.61, 0.41, and 0.30 mu g m(-3) h(-1) in autumn, summer, spring, and winter, respectively. Despite the similar concentrations of aromatic and aliphatic OOMs, the former had lower volatilities and, therefore, showed higher contributions (46 %-62 %) to SOA than the latter (14 %-32 %). By contrast, monoterpene OOMs and isoprene OOMs, limited by low abundances or high volatilities, had low contributions of 8 %-12 % and 3 %-5 %, respectively. Overall, our results improve the understanding of the concentration, chemical composition, seasonal variation, and potential atmospheric impacts of OOMs, which can help formulate refined restriction policy specific to SOA control in urban areas.Peer reviewe

Sources and sinks driving sulfuric acid concentrations in contrasting environments : implications on proxy calculations

Sulfuric acid has been shown to be a key driver for new particle formation and subsequent growth in various environments, mainly due to its low volatility. However, direct measurements of gas-phase sulfuric acid are oftentimes not available, and the current sulfuric acid proxies cannot predict, for example, its nighttime concentrations or result in significant discrepancies with measured values. Here, we define the sources and sinks of sulfuric acid in different environments and derive a new physical proxy for sulfuric acid to be utilized in locations and during periods when it is not measured. We used H2SO4 measurements from four different locations: Hyytiala, Finland; Agia Marina, Cyprus; Budapest, Hungary; and Beijing, China, representing semi-pristine boreal forest, rural environment in the Mediterranean area, urban environment and heavily polluted megacity, respectively. The new proxy takes into account the formation of sulfuric acid from SO2 via OH oxidation and other oxidation pathways, specifically via stabilized Criegee intermediates. The sulfuric acid sinks included in the proxy are its condensation sink (CS) and atmospheric clustering starting from H2SO4 dimer formation. Indeed, we found that the observed sulfuric acid concentration can be explained by the proposed sources and sinks with similar coefficients in the four contrasting environments where we have tested it. Thus, the new proxy is a more flexible and an important improvement over previous proxies. Following the recommendations in this paper, a proxy for a specific location can be derived.Peer reviewe