Journal of Geophysical Research: Atmospheres最新文献

Religious burning (RB) has been identified as a major source of atmospheric aerosols on the Qinghai-Tibet Plateau. However, there is limited understanding of the detailed chemical composition, size distribution, and optical properties of RB aerosols in this region. To characterize these important aerosol properties, ambient PM_2.5 and size resolved aerosols from RB emissions in Lhasa were collected during summer 2019. Organic functional group (OFG) and inorganic ion composition was measured using Fourier transform infrared spectroscopy and ion chromatography, respectively. The ambient PM_2.5 was dominated by organic components, with the OFG concentrations significantly higher during religious events, reflecting the substantial impact of RB emissions on local air quality. The RB aerosols were characterized by high fractions of alkane (34%), hydroxyl (29%), and carboxylic acid (13%) groups, with peak mass in the accumulation mode (0.56–1.00 μm). The high abundance of hydroxyl group and the size distribution pattern suggested that the RB aerosols were formed from volatilization of fuel materials followed by unaltered condensation, a process that may be unique to the low-temperature, low-oxygen burning in the scattered burners at the temples. The absorption coefficient of RB aerosols showed similar size distribution to the mass size distribution, but the absorption Ångström exponent displayed the lowest value in the 0.56–1.00 μm size mode. This specific size distribution aligned with the mass fraction of carboxylic acids and mirrored the mass proportion of alkanes, suggesting that smaller and larger particles were enriched with substances that have higher light-absorbing capabilities.

Weather features, such as extratropical cyclones, atmospheric rivers (ARs), and fronts, contribute to substantial amounts of precipitation globally and are associated with different precipitation characteristics. However, future changes in these characteristics, as well as their representation in climate models, remain uncertain. We attribute 6-hourly accumulated precipitation to cyclones, moisture transport axes (AR-like features), fronts, and cold air outbreaks, and the combinations thereof in 10 ensemble members of the CESM2-LE between 1960 and 2100 under the SSP3-7.0 scenario. We find that, despite some biases in both precipitation and weather features, CESM2-LE adeptly represents the precipitation characteristics associated with the different combinations of weather features. The combinations of weather features that contribute most to precipitation in the present climate also contribute the most to future changes, both due to changes in intensity as well as frequency. While the increase in precipitation intensity dominates the overall response for total precipitation in the storm track regions, the precipitation intensity for the individual weather features does not necessarily change significantly. Instead, approximately half of the increase in precipitation intensity in the storm track regions can be attributed to a higher occurrence of the more intensely precipitating combinations of weather features, such as the co-occurrence of extratropical cyclones, fronts, and moisture transport axes.

We investigate the synoptic and mesoscale dynamics of two wet and two dry cold surges in January 2021 using a combination of observations, reanalysis, and convective-scale model forecasts from the Met Office Unified Model (MetUM). We focus on the wet surges, and particularly the wettest days which are locally extreme over Singapore and the surrounding region (i.e., the daily mean and area-averaged rainfall over 20 years exceeds the 99th percentile). On the large scale, the wet surges are characterized by an anomalously strong anticyclone over Siberia prior to their onset. The anticyclone and resultant surge winds are stronger than those of the dry surges. There is also a relatively moist (dry) environment prior to the onset of the wet (dry) surges, with the Madden-Julian Oscillation (MJO) being in Phase 3 (Phase 6). On the mesoscale, the combination of the cold surge and a local tropical low produce strong, moist north-easterly winds and convection over the Singapore region. The equatorward advection of positive anomalies of equivalent potential temperature resembles a weak gravity-current-like structure at its head, although the spatial scale is much too large for a gravity current. There is a moist bias in the model forecasts, although the precipitation is underestimated regionally during the wet surges and particularly on the extreme rainfall days. Overall, the model forecasts perform well synoptically but not in the details of mesoscale convection.

Methane (CH₄) is the second most abundant greenhouse gas and affects the Earth's radiative balance. In some regions, the methane burden and budget are still not well understood due to the lack of in situ observations, especially vertical profile observations. Here, we present the first high-resolution aircraft-based tropospheric vertical profiles of CH₄ across the Indian subcontinent. Observations show significant variability, with the largest variability seen in the Indo-Gangetic Plain (IGP) during post-monsoon (September). The IGP also shows the highest concentrations and a peak in the boundary layer. By contrast, observations over western India show lower variability, especially during the Asian Summer Monsoon (ASM) (July). During ASM, when CH₄ emissions peak, the vertical updraft of CH₄ and other tracers is observed, leading to a peak between 4 and 5 km. During winter, the peak occurs in the boundary layer, and a decrease with altitude is observed. Model simulations slightly overestimate CH₄ at the surface during some seasons but underestimate it at higher altitudes during all seasons. Integrated over the observed column, model simulations slightly underpredict CH₄ (0.5%–3.1%) during all seasons. Calculations made using the observed CO/CH₄ enhancement ratios show that in addition to anthropogenic fossil fuel emissions, other sources, such as rice cultivation and wetlands, need to be considered to reproduce the observed CH₄ concentrations.

Over the past decades, various experimental and numerical model studies have indicated cooling trend in the mesosphere and lower thermosphere (MLT), while the magnitude of the trend varies noticeably. Previous studies using the lidar observations derived the temperature trends and solar responses solely from the traditional nocturnal measurements. While these archived results are more or less in agreement with modeling studies, one of the main uncertainties in these studies is the potential biases induced by the trends of the diurnal tide forced in the lower atmosphere, and that of the in situ exothermal reactions involving the photolysis. In the MLT, the diurnal tide has significant seasonal variations, considerable amplitude and is one of the dominant dynamic sources. However, its potential effects in the trend studies have rarely been discussed. In this paper, we present and compare the long-term temperature trends in the upper mesosphere utilizing the daily mean and nightly mean temperature profiles measured by a Sodium (Na) Doppler lidar at midlatitude. The system was operating routinely in full diurnal cycles between 2002 and 2017, obtaining a unique multi-year temperature data set. A customized multi-linear regression (MLR) model is applied to determine the linear trends and the other fitting parameters, such as ENSO and solar F10.7 responses in the upper mesosphere. This study indicates the daily mean cooling trend between 84 and 98 km is larger than that of nightly mean trend by ∼−1 K/decade, while differences in the solar response are within the fitting uncertainties.

We use measurements of trace gases from the Microwave Limb Sounder and polar stratospheric clouds (PSCs) from the Cloud-Aerosol Lidar with Orthogonal Polarization to investigate how the extraordinary stratospheric water vapor enhancement from the 2022 Hunga eruption affected polar processing during the 2023 Antarctic winter. Although the dynamical characteristics of the vortex itself were generally unexceptional, the excess moisture initially raised PSC formation threshold temperatures above typical values. Cold conditions, especially in early July, prompted ice PSC formation and unusually severe irreversible dehydration at higher levels (500–700 K), while atypical hydration occurred at lower levels (380–460 K). Heterogeneous chemical processing was more extensive, both vertically (up to 750–800 K) and temporally (earlier in the season), than in prior Antarctic winters. The resultant HCl depletion and ClO enhancement redefined their previously observed ranges at and above 600 K. Albeit unmatched in the satellite record, the early-winter upper-level chlorine activation was insufficient to induce substantial ozone loss. Chlorine activation, denitrification, and dehydration processes ran to completion by July/August, with trace gas evolution mostly following the climatological mean thereafter, but with chlorine deactivation starting slightly later than usual. While cumulative ozone losses at 410–550 K were relatively large, probably because of the delayed chlorine deactivation, they were not unprecedented. Thus, ozone depletion was unremarkable throughout the lower stratosphere. Although Hunga enhanced PSC formation and chemical processing in early winter, saturation of lower stratospheric denitrification, dehydration, and chlorine activation (as is typical in the Antarctic) prevented an exceptionally severe ozone hole in 2023.

Hydration of the stratosphere by tropopause-overshooting convection has received increasing interest due to the extreme concentrations of water vapor that can result and, ultimately, the climate warming potential such hydration provides. Previous work has recognized the importance of numerous dynamic and physical processes that control stratospheric water vapor delivery by convection. This study leverages recent comprehensive observations from the NASA Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) field campaign to determine the frequency at which each process operates during real events. Specifically, a well-established analysis technique known as tracer-tracer correlation is applied to DCOTSS observations of ozone, water vapor, and potential temperature to identify the occurrence of known processes. It is found that approximately half of convectively-driven stratospheric hydration samples show no indication of significant air mass transport and mixing, emphasizing the importance of ice sublimation to stratospheric water vapor delivery. Furthermore, the temperature of the upper troposphere and lower stratosphere environment and/or overshoot appears to be a commonly active constraint, since the approximate maximum possible water vapor concentration that can be reached in an air mass is limited to the saturation mixing ratio when ice is present. Finally, little evidence of relationships between dynamic and physical processes and their spatial distribution was found, implying that stratospheric water vapor delivery by convection is likely facilitated by a complex collection of processes in each overshooting event.

Proteinaceous matter (PrM) is a substantial component of bioaerosols. Although numerous studies have examined the characteristics and sources of PrM in the atmosphere, its interactions with atmospheric oxidants remain uncertain. A 1-year observation of PrM characteristics in PM_2.5 was performed in both urban Nanchang (eastern China) and suburban Guiyang (southwestern China), respectively. Glycine was the dominant free amino acid (FAA) species in urban Nanchang. In contrast, proline dominated both total free amino acids (FAAs) and total combined amino acids (CAAs) in suburban Guiyang. We found that oxidative degradation can significantly promote the release of FAAs, especially glycine, from CAAs in Nanchang. The controlled experiment on protein oxidation by hydroxyl radical suggested that the contribution of free glycine to the total FAA fraction tended to increase during the oxidative degradation of CAAs, supporting the predominance of glycine in FAAs in Nanchang and most previous observations. The composition of FAAs was mainly influenced by primary sources in suburban Guiyang with weak atmospheric degradation of PrM. These results suggest that the degradation of aerosol PrM by atmospheric oxidants can be responsible for the difference in FAA composition between the biosphere and the atmosphere, and also imply that the oxidative degradation of aerosol PrM may be a potential source of secondary organic nitrogen compounds in aerosols. Thus, this study can improve the current understanding of the composition characteristics of PrM in the biosphere and the atmosphere, as well as the liquid phase reactions of proteinaceous compounds with atmospheric oxidants.

The Bay of Bengal summer monsoon (BOBSM) is the most prominent branch of the Asian summer monsoon system, which exhibits complex interannual variability. While previous studies have focused on the onset conditions of the BOBSM, less attention has been paid to the retreat of the BOBSM. In this study, we propose an index to measure BOBSM retreat, based on the mean zonal wind field at 850 hPa during the summer-to-winter monsoon transitions. By analyzing the climatic characteristics and interannual variability of the BOBSM retreat using this index, we find that BOBSM retreat exhibits significant interannual variability, which is closely related to the occurrence of Indian Ocean Dipole (IOD) events. Statistically, when a positive IOD event takes place in the boreal autumn season, the retreat of the summer monsoon occurs earlier correspondingly. Conversely, the retreat is delayed when a negative IOD event occurs.

Modeling atmospheric black carbon (BC) aerosol optical properties remains largely uncertain due to their complex mixing states, nonsphericity, and heterogeneity of coating distribution. Although there exist numerical models with realistic BC morphologies, these models are mostly limited to particle-scale studies and have not been coupled to large-scale atmospheric or climate models. In this study, a multidimensional parameterization scheme is developed by an accurate numerical algorithm for BC optical property calculation in global climate models, by incorporating their mixing state and nonspherical structure as well as heterogeneous coating distribution. The scheme was coupled and tested with the Community Atmosphere Model version 6 (CAM6) by a weighted averaging algorithm for individual particles and integration for particle ensembles. The simulation results indicate that BC morphology has a limited influence on the aerosol absorption cross section (C_abs), and the differences in C_abs between irregularly coated fractal aggregates and ideal core-shell spherical (CS) counterparts are ∼3% on average. However, the relative positions between the BC core and coating parts may introduce C_abs variations of up to 69% as compared with the CS results. The BC mixing state introduce ∼20% relative variations in the global average aerosol absorption optical depth, which is comparable to that of heterogeneity of coating distribution and three times greater than that of particle nonsphericity. Furthermore, the normalized mean biases of modeled single scattering coalbedo (1−SSA, i.e., the ratio of absorption to extinction) compared to those observed in BC-rich regions are reduced by 20%∼80% when applying our new parameterization in CAM6.