[Characteristics of Light Absorption, Sources, and Seasonal Variation of Atmospheric Brown Carbon in Northern Nanjing].

Brown carbon (BrC) refers to a group of organic compounds in fine atmospheric particles (PM2.5) that are able to absorb light in the ultraviolet and visible range. They have a significant impact on the visibility of air and on the earth's climate. In this study, we used a black carbon analyzer (Model AE33) to conduct field measurements in northern suburban Nanjing from March 2021 to February 2022. We measured the light absorption coefficients of BrC in PM2.5 and quantified the contributions of primary (BrCpri) and secondary brown carbon (BrCsec) in BrC by using the minimum correlation method (MRS), combined with the backward trajectories,potential source contribution function (PSCF) analysis, and diurnal patterns to analyze the seasonal characteristics of BrC. The results showed that the annual average light absorption of BrC was(7.76±7.17)Mm-1 (at 370 nm), and its contribution to the total aerosol light absorption was (22.0±8.8)%. BrC light absorption at different wavelengths all showed a U-shape seasonal variation of high in spring and winter and low in summer and fall. MRS analysis showed that the annual average contributions of BrCpri and BrCsec were (62.9±21.4)% and (37.1±21.4)% (at 370 nm), respectively; however, the contribution of BrCsec increased with the increase in wavelength, and it became dominant in longer wavelengths such as 660 nm. Backward trajectory and PSCF analysis showed that BrC was heavily influenced by air masses from the sea in spring, summer, and fall but was influenced greatly by local and regional continental emissions in winter. Traffic emissions in spring, summer, and fall were more intense to contribute to BrCpri than that in winter, whereas coal and biomass combustion had a greater impact on BrCpri in winter. Detailed analysis revealed that gas-phase photochemistry and aqueous chemistry had different influences on BrCsec formation in different seasons. It was mainly from gas-phase photochemistry in summer but was dominated by aqueous process in winter; both processes, however, were important pathways to BrCsec in spring and fall.

[Characteristics and Sources of Nitrated Phenols in Atmospheric Fine Particles of Northern Suburban Nanjing].

Nitrated phenols are a group of nitrogen-containing organics ubiquitously present in ambient air, which are also important components of atmospheric light-absorbing organic matter (brown carbon) that have significant impacts on climate change, air quality, and human health. In this study, we collected a total of 265 daily filter samples of fine particles (PM2.5) in northern suburban Nanjing from March 2019 to January 2020. We used ultra-high performance liquid chromatography-mass spectrometry (UHPLC-MS) to detect and quantify eight nitrated phenolic species. The results showed that the average annual concentration of total nitrated phenols in the sampling site was 18.77 ng·m-3, and the average concentrations in spring, summer, autumn, and winter were 16.82, 8.59, 17.28, and 44.79 ng·m-3, respectively. Such concentrations were obviously higher than those determined in other countries but were similar to those in domestic cities, such as Jinan. 4-Nitrophenol was the most abundant nitrated phenol, followed by 4-nitrocatechol and 2-methoxy-5-nitrophenol. Correlation analysis showed that 3-nitrosalicylic acid was from a specific source different from that of other species. Finally, we used a positive matrix factorization model to quantify the source contributions of nitrated phenols. The major sources were vehicle emissions (32%), mixed coal and biomass burning emissions (44%), and industrial emissions (24%). The mixed coal and biomass burning emissions were dominant in autumn and winter. The mass fraction of 3-nitrosalicylic acid in the factor of industrial emissions was>90%, consistent with the results of the correlation analysis. Overall, this study provides valuable insights into the understanding of concentrations, characteristics, and sources of atmospheric nitrated phenols in ambient air.

[Aqueous-phase Oxidation of Dissolved Organic Matter (DOM) from Extracts of Ambient Aerosols].

Recently, a large number of laboratory studies have focused on the aqueous-phase photochemistry of single organic compound in atmospheric condensed phases, yet few studies have been conducted on the aqueous-phase photochemical oxidation of real-world complex dissolved organic matter (DOM). Therefore, in this work, we report experimental results for the photochemical oxidation of DOM extracts from ambient fine aerosol samples upon direct photolysis or against OH oxidation, under both simulated sunlight and ultraviolet irradiation conditions. The products at different stages of photolysis were analyzed via UV-vis and spectroscopy and soot-particle aerosol mass spectrometry (SP-AMS) to investigate their optical and chemical characteristics. The results demonstrate the effective degradation of DOM under UV irradiation, and the f44 values of the corresponding products aremuch lower than under sunlight irradiation. A variety of carboxylic acids were generated during liquid-phase photolysis, and oxalic acid was found to be the most abundant. The light absorbance and concentration of HULIS did not change significantly under sunlight illumination; however, under UV and UV+·OH conditions, the concentration of HULIS increased continuously with reaction time. The HULIS concentration at 23 h was approximately four times the initial value, indicating the formation of brown carbon species with carboxyl, hydroxyl, and aromatic and other functional groups. Our results show that the increase in light absorptivity and formation rate of brown carbon from DOM are limited when aqueous-phase oxidation occurs under sunlight illumination. In comparison, DOM can constantly decompose into HULIS or small molecules under ultraviolet light illumination, and the light absorptivity of the remaining organic matter may be relatively high, resulting in final products with a high unit mass absorption efficiency (MAE). We have investigated the aqueous-phase oxidation of actual filter extracts for the first time, and our results provide valuable insights to the formation of air pollution complexes.

[Analysis of Water Soluble Organic Aerosol in Spring PM2.5 with Soot Particle Aerosol Mass Spectrometry (SP-AMS)].

To investigate the chemical composition and pollution characteristics of spring fine particles (PM2.5) in Changzhou, a total of 84 PM2.5 samples were collected from March 1st to May 30th, 2017. We measured and analyzed conventional components, such as water-soluble ions (WSIIs) and carbonaceous components (OC and EC). The water-soluble organic aerosol (WSOA) was also analyzed by an aerodyne soot particle aerosol mass spectrometer (SP-AMS). During the sampling period, the average daily PM2.5 concentration was 101.97 µg·m-3, with more than 73.8% sampling days exceeding the Target-2 standard of the national ambient air quality standard of China. The air quality during the sampling period was dominated by light, moderate, and heavy pollution, accounting for 39.3%, 21.4%, and 13.1% of the total days, respectively. The total WSIIs accounted for 39.86% of PM2.5 mass, of which secondary ions (SO42-, NH4+, and NO3-) accounted for 81.85% of the total WSIIs. The slope of the linear fitted line of the anion and cation charge balance (AE/CE) was greater than 1 (1.09), which indicated that PM2.5 was weakly acidic. The average OC/EC ratio was 2.53, indicating that PM2.5 was influenced by the secondary conversion. WSOA included CxHy+(32.1%), CxHyO+(30.4%), CxHyO2+(25.4%), and HyO+(4.7%) identified by SP-AMS. The average oxygen-to-carbon (O/C), hydrogen-to-carbon (H/C), nitrogen-to-carbon (N/C), and organic matter-to-organic carbon (OM/OC) ratios of the WSOA were 0.72, 1.53, 0.04, and 2.15, respectively. Higher O/C indicated higher contributions from secondary photochemical reaction conversion in spring. Positive matrix factorization (PMF) analysis for AMS mass spectra of WSOA identified three sources, namely hydrocarbon-like (HOA), semi-volatile oxygenated OA (SVOOA)-biomass burning OA (BBOA), and low-volatility oxygenated OA (LVOOA), which on average accounted for 18.4%, 34.1%, and 47.4% of the total WSOA, respectively.

Quantum control of electron wave packet during high harmonic process of H2(+) in a combination of a circularly polarized laser field and a Terahertz field.

By solving a two-dimensional time-dependent Schrödinger equation we investigate high harmonic generation (HHG) and isolated attosecond pulse generation for the H2+ molecular ion in a circularly polarized laser pulse combined with a Terahertz (THz) field. The harmonic intensity can be greatly enhanced and a continuum spectrum can be obtained when a THz field is added. The HHG process is studied by the semi-classical three-step model and the time-frequency analysis. Our studies show that only short trajectories contribute to HHG. Furthermore, we present the temporal evolution of the probability density of electron wave packet, which perfectly shows a clear picture of the electron's two-time recombination when a THz field is added, and it is the main mechanism of HHG. By superposing the harmonics in the range of 216-249 eV, an isolated attosecond pulse with a duration of about 69 attoseconds can be generated.