Free Troposphere Research Articles

A Dynamical Interpretation of the Intensification of the Winter North Atlantic Jet Stream in Reanalysis

Abstract Jet streams play an important role in determining weather variability and extremes. A better understanding of the mechanisms driving long-term changes in the jet is essential to successfully anticipate extreme meteorological events. This study analyzes the intensification trend of the North Atlantic jet using the ERA5 reanalysis and investigates the dynamical mechanisms involved. The results highlight the importance of an increase in diabatic heating in the free troposphere below the jet entrance over the Gulf Stream sector. This change in diabatic heating modifies the jet directly and produces a local intensification and a slight poleward shift. A two-dimensional frontal-geostrophic model illustrates this mechanism by considering the enhanced diabatic heating associated with the baroclinic growth of extratropical cyclones. The change in diabatic heating also affects the jet indirectly by increasing the mean baroclinicity and subsequent eddy momentum flux convergence. This indirect mechanism has also an effect downstream, where there is an acceleration of the jet core and reduced westerlies along the flanks, reducing the width of the jet. An idealized warming experiment confirms this mechanism by determining the jet response downstream of an idealized land–sea contrast. Finally, using a single-model ensemble of fully coupled climate simulations, we show that the differences in the evolution of the North Atlantic jet are related to the latitude of the increase in baroclinicity, which has a large spread. What emerges from the model hierarchy is a consistent dynamical chain of mechanisms associated with the intensification trend of the North Atlantic jet stream.

Future Changes in the Vertical Structure of Severe Convective Storm Environments over the U.S. Central Great Plains

Abstract The effect of warming on severe convective storm potential is commonly explained in terms of changes in vertically integrated (“bulk”) environmental parameters, such as CAPE and 0–6-km shear. However, such events are known to depend on the details of the vertical structure of the thermodynamic and kinematic environment that can change independently of these bulk parameters. This work examines how warming may affect the complete vertical structure of these environments for fixed ranges of values of high CAPE and bulk shear, using data over the central Great Plains from two high-performing climate models (CNRM and MPI). To first order, projected changes in the vertical sounding structure are consistent between the two models: the environment warms approximately uniformly with height at constant relative humidity, and the shear profile remains relatively constant. The boundary layer becomes slightly drier (−2% to 6% relative humidity) while the free troposphere becomes slightly moister (+1% to 3%), with a slight increase in moist static energy deficit aloft with stronger magnitude in CNRM. CNRM indicates enhanced low-level shear and storm-relative helicity associated with stronger hodograph curvature in the lowest 2 km, whereas MPI shows near-zero change. Both models strongly underestimate shear below 1 km compared to ERA5, indicating large uncertainty in projecting subtle changes in the low-level flow structure in climate models. The evaluation of the net effect of these modest thermodynamic and kinematic changes on severe convective storm outcomes cannot be ascertained here but could be explored in simulation experiments. Significance Statement Severe thunderstorms and tornadoes cause substantial damage and loss of life each year, which raise concerns about how they may change as the world warms. We typically use a small number of common atmospheric parameters to understand how these localized events may change with climate change. However, climate change may alter the weather patterns that produce these events in ways not captured by these parameters. This work examines how climate change may alter the complete vertical structure of temperature, moisture, and wind and discusses the potential implications of these changes for future severe thunderstorms and tornadoes.

Radiative Feedback From Dry Environmental Air Accelerates Tropical Cyclogenesis

AbstractA number of recent studies have highlighted how radiative feedback from clouds accelerates tropical cyclone (TC) development by amplifying spatial gradients in radiative heating. This study extends this work by examining how spatial gradients in free tropospheric moisture influence TC development through their impact on environmental radiative heating. We conduct a series of idealized model experiments in which only the longwave radiative heating due to water vapor is modified in the environmental region outside of the TC area. These experiments demonstrate that a vortex in a drier environmental free troposphere experiences faster development. Moreover, weaker vortices actually require a dry environmental free troposphere to develop. The accelerated genesis mainly results from a stronger spatial gradient in moisture‐induced radiative heating, which enhances energy convergence through a stronger transverse circulation. These results highlight a potentially important and overlooked role of dry air in facilitating TC genesis.

Sources and Variability of Greenhouse Gases over Greece

This study provides an overview of the atmospheric drivers of climate change over Greece (Eastern Mediterranean), focusing on greenhouse gases (GHG: carbon dioxide, CO2; methane, CH4; etc.). CO2 in Greece is mostly produced by energy production, followed by transport, construction, and industry. Waste management is the largest anthropogenic source of methane, accounting for 47% of total CH4 emissions, surpassing emissions from the agricultural sector in 2017, while the energy sector accounts for the remaining 10.5%. In situ simultaneous observations of GHG concentrations in Greece conducted at three sites with different topologies (urban background; Athens, regional background; Finokalia and free troposphere; and Helmos) during the last 5 years (2019–2023) showed increasing trends of the order of 2.2 ppm·yr−1 and ~15 ppb·yr−1 for CO2 and CH4, respectively, in line with the global trends. These increasing trends were found from both ground-based and satellite-based remote-sensing observations. Finally, during the lockdown period due to the COVID-19 global pandemic, a 58% reduction in CO2 levels was observed in the urban background site of Athens after subtracting the regional background levels from Finokalia, while the respective reduction in CH4 was of only the order of 15%, highlighting differences in emission sources.

Troposphere–stratosphere-integrated bromine monoxide (BrO) profile retrieval over the central Pacific Ocean

Abstract. Bromine monoxide (BrO) is relevant to atmospheric oxidative capacity, affecting the lifetime of greenhouse gases (i.e., methane, dimethylsulfide) and mercury oxidation. However, measurements of BrO radical vertical profiles are rare, and BrO is highly variable. As a result, the few available aircraft observations in different regions of the atmosphere are not easily reconciled. Autonomous multi-axis differential optical absorption spectroscopy (MAX-DOAS) instruments placed at remote mountaintop observatories (MT-DOAS) present a cost-effective alternative to aircraft, with the potential to probe the climate-relevant yet understudied free troposphere more routinely. Here, we describe an innovative full-atmosphere BrO and formaldehyde (HCHO) profile retrieval algorithm using MT-DOAS measurements at Mauna Loa Observatory (MLO – 19.536° N, 155.577° W; 3401 m a.s.l.). The retrieval is based on time-dependent optimal estimation and simultaneously inverts 190+ individual BrO (and formaldehyde, HCHO) SCDs (slant column densities; SCD = dSCD + SCDRef) from solar stray light spectra measured in the zenith and off-axis geometries at high and low solar zenith angles (92° > SZA > 30°) to derive BrO concentration profiles from 1.9 to 35 km with 7.5 degrees of freedom (DoFs). Two case study days are characterized by the absence (26 April 2017, base case) and presence of a Rossby-wave-breaking double tropopause (29 April 2017, RW-DT case). Stratospheric-BrO vertical columns are nearly identical on both days (VCD = (1.5 ± 0.2) × 1013 molec. cm−2), and the stratospheric-BrO profile peaks at a lower altitude during the RW-DT (1.6–2.0 DoFs). Tropospheric-BrO VCDs increase from (0.70 ± 0.14) × 1013 molec. cm−2 (base case) to (1.00 ± 0.14) × 1013 molec. cm−2 (RW-DT) owing to a 3-fold increase in BrO in the upper troposphere (1.7–1.9 DoFs). BrO at MLO increases from (0.23 ± 0.03) pptv (base case) to (0.46 ± 0.03) pptv (RW-DT) and is characterized by an added time resolution (∼ 3.8 DoFs). Up to (0.9 ± 0.1) pptv BrO is observed above MLO in the lower free troposphere in the absence of the double tropopause. We validate the retrieval using aircraft BrO profiles and in situ HCHO measurements aboard the NSF/NCAR GV aircraft above MLO (11 January 2014) that establish BrO peaks around 2.4 pptv above 13 km in the upper troposphere–lower stratosphere (UTLS) during a similar RW-DT event (0.83 × 1013 molec. cm2 tropospheric-BrO VCD above 2 km). The tropospheric-BrO profile measured using MT-DOAS (RW-DT case) and using the aircraft agree well (after averaging-kernel smoothing). Furthermore, these tropospheric-BrO profiles over the central Pacific Ocean are found to closely resemble those over the eastern Pacific Ocean (2–14 km) and are in contrast to those over the western Pacific Ocean, where a C-shaped tropospheric-BrO profile shape has been observed.

The Pivotal Role of Heavy Terpenes and Anthropogenic Interactions in New Particle Formation on the Southeastern Qinghai-Tibet Plateau.

Aerosol particles originating from the Qinghai-Tibet Plateau (QTP) readily reach the free troposphere, potentially affecting global radiation and climate. Although new particle formation (NPF) is frequently observed at such high altitudes, its precursors and their underlying chemistry remain poorly understood. This study presents direct observational evidence of anthropogenic influences on biogenic NPF on the southeastern QTP, near the Himalayas. The mean particle nucleation rate (J1.7) is 2.6 cm-3 s-1, exceeding the kinetic limit of sulfuric acid (SA) nucleation (mean SA: 2.4 × 105 cm-3). NPF is predominantly driven by highly oxygenated organic molecules (HOMs), possibly facilitated by low SA levels. We identified 1538 ultralow-volatility HOMs driving particle nucleation and 764 extremely low-volatility HOMs powering initial particle growth, with mean total concentrations of 1.5 × 106 and 3.7 × 106 cm-3, respectively. These HOMs are formed by atmospheric oxidation of biogenic precursors, unexpectedly including sesquiterpenes and diterpenes alongside the commonly recognized monoterpenes. Counterintuitively, over half of HOMs are organic nitrates, mainly produced by interacting with anthropogenic NOx via RO2+NO terminations or NO3-initiated oxidations. These findings advance our understanding of NPF mechanisms in this climate-sensitive region and underscore the importance of heavy terpene and NOx-influenced chemistry in assessing anthropogenic-biogenic interactions with climate feedbacks.

Extreme wildfires over northern Greece during summer 2023 – Part A: Effects on aerosol optical properties and solar UV radiation

In Mediterranean countries, such as Greece, the frequency of forest fires has increased in recent years, primarily due to the widespread impacts of climate change. At the end of August 2023, Greece experienced a record-breaking heatwave that triggered severe wildfire incidents, significantly impacting the atmospheric conditions of several cities, among them Thessaloniki. A significant number of wildfires occurred in northern Greece (Evros), burning thousands of hectares of the protected Dadia forest (Natura 2000) and releasing a significant load of smoke into the atmosphere. According to the European Strategy Forum on Research Infrastructures (ESFRI) a total area of 90,000ha was burnt collectively by the Evros extreme wildfires during August 2023. The emissions led to severely adverse air pollution conditions, causing reduced visibility across an extended eastern Mediterranean region for several days. In this work, we analyze the influence of the transported biomass burning particles on the aerosol properties in the free troposphere, as well as on the surface UV radiation levels over Thessaloniki during the last week of August 2023. The transported smoke plume was detected over the Laboratory of Atmospheric Physics (LAP) in Thessaloniki, approximately 240 km away from the burning area, from August 22nd to the 25th. During this period, the presence of smoke led to exceptionally increased levels of aerosol optical depth (AOD), reaching up to 3.4 at 340nm (the highest ever recorded in Thessaloniki), as well as high Ångström exponent (AE) values, peaking at 2.4 for the 440–870nm range, followed by high Fine Mode Fractions (FMFs), indicating the prevalence of fine-mode smoke aerosol particle. Moreover, during the event, the presence of the biomass burning aerosols led to a strong attenuation of the solar UV irradiance by up to 90 %, reaching unprecedented levels, similar of a solar eclipse. The primary goal of this study is to highlight the extensive impacts that wildfires have, which are anticipated to increase in frequency in the near future, due to the predicted rise in the rate of occurrence of summer heatwaves especially for Mediterranean areas and specifically for Greece. Furthermore, the great value of the synergistic monitoring of the event with ground-based remote sensing instrumentation, along with satellite aerosol observations and modeling tools, is made prominent.

Bridging gas and aerosol properties between the northeastern US and Bermuda: analysis of eight transit flights

Abstract. The western North Atlantic Ocean is strongly influenced by continental outflow, making it an ideal region to study the atmospheric transition from a polluted coastline to the marine environment. Utilizing eight transit flights between the NASA Langley Research Center (LaRC) in Hampton, Virginia, and the remote island of Bermuda from NASA's Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE), we examine the evolution of trace gas and aerosol properties off the US East Coast. The first pair of flights flew along the wind trajectory of continental outflow, while the other flights captured a mix of marine and continental air mass sources. For measurements within the boundary layer (BL), there was an offshore decline in particle N<100 nm, N>100 nm, CH4, CO, and CO2 concentrations, all leveling off around ∼900 km offshore from the LaRC. These trends are strongest for the first pair of flights. In the BL, offshore declines in organic mass fraction and increases in sulfate mass fraction coincide with increasing hygroscopicity based on f(RH) measurements. Free troposphere measurements show a decline in N<100 nm, but other measured parameters are more variable when compared to the prominent offshore gradients seen in the BL. Pollution layers exist in the free troposphere, such as smoke plumes, that can potentially entrain into the BL. This work provides detailed case studies with a broad set of high-resolution measurements to further our understanding of the transition between continental and marine environments.

Unraveling atmospheric mercury dynamics at Mauna Loa through the isotopic analysis of total gaseous mercury

Our investigation seeks to uncover the intricate nature of mercury dynamics in the free troposphere through analysis of the isotopic composition of total gaseous elemental mercury (TGM) at the high altitude Mauna Loa Observatory (MLO, 3397 m) in Hawaii, USA. By focusing on this unique site, we aim to provide essential insights into the behavior and cycling of mercury, contributing valuable data to a deeper understanding of its global distribution and environmental impacts. Forty-eight hours of TGM sampling from January to September 2022 revealed significant variations in δ202Hg (−1.86 % to −0.32 %; mean = −1.17 ± 0.65 %, 2 SD, n = 34) and small variations in Δ199Hg (−0.27 % to 0.04 %; mean = −0.13 ± 0.14 %, 2 SD, n = 34) and Δ200Hg (−0.20 % to 0.06 %; mean = −0.05 ± 0.13 %, 2 SD, n = 34). During the sampling period, GEM was negatively correlated with gaseous oxidized mercury (GOM). However, the GOM/GEM ratio was not −1, suggesting that GEM oxidation and subsequent scavenging occurred previously. The δ202Hg isotopic compositions of TGM at MLO were different from those of reported values of high-altitude mountains; the δ202Hg of TGM at MLO was lower than the isotopic ratios that were obtained from other mountain regions. The unique atmospheric conditions at Mauna Loa, with (upslope winds during the day and downslope winds at night, likely result in the) possibly mixing of GEMs from terrestrial (and possibly oceanic GEM emission) sources with and tropospheric sources, influencing and affect the isotopic composition. During the late summer to early fall (September 14–28), negative correlations were found between relative humidity and GOM and between particle number concentrations and Δ199Hg, indicating the gas-to-particle partitioning of the atmospheric mercury during this period. This study will improve our understanding on mercury dynamics of marine origin and high altitudes and shed light on its complex interactions with environmental factors.

Atmospheric Bases-Enhanced Iodic Acid Nucleation: Altitude-Dependent Characteristics and Molecular Mechanisms.

Iodic acid (IA), the key driver of marine aerosols, is widely detected within the gas and particle phases in the marine boundary layer (MBL) and even the free troposphere (FT). Although atmospheric bases like dimethylamine (DMA) and ammonia (NH3) can enhance IA particles formation, their different efficiencies and spatial distributions make the dominant base-stabilization mechanisms of forming IA particles unclear. Herein, we investigated the IA-DMA-NH3 nucleation system through quantum chemical calculations at the DLPNO-CCSD(T)/aug-cc-pVTZ(-PP)//ωB97X-D/6-311++G(3df,3pd) + aug-cc-pVTZ-PP level of theory and cluster dynamics simulations. We provide molecular-level evidence that DMA and NH3 can jointly stabilize the IA clusters. The formation rates of IA clusters initially decline before rising from the MBL to the FT, owing to variations in mechanism. In the MBL, IA-DMA nucleation predominates, while the contribution of IA-DMA-NH3 synergistic nucleation cannot be overlooked in polar and NH3-polluted regions. In the lower FT, IA-DMA-NH3 nucleation prevails, whereas in the upper FT, IA-NH3 nucleation dominates. The efficiency of IA-DMA-NH3 nucleation is comparable to that of IA-iodous acid nucleation in the MBL and sulfuric acid-NH3 nucleation in the FT. Hence, the IA-DMA-NH3 mechanism holds promise for revealing the missing sources of tropospheric IA particles.

Biological and dust aerosols as sources of ice-nucleating particles in the eastern Mediterranean: source apportionment, atmospheric processing and parameterization

Abstract. Aerosol–cloud interactions in mixed-phase clouds (MPCs) are one of the most uncertain drivers of the hydrological cycle and climate change. A synergy of in situ, remote-sensing and modelling experiments were used to determine the source of ice-nucleating particles (INPs) for MPCs at Mount Helmos in the eastern Mediterranean. The influences of boundary layer turbulence, vertical aerosol distributions and meteorological conditions were also examined. When the observation site is in the free troposphere (FT), approximately 1 in ×106 aerosol particles serve as INPs around −25 °C. The INP abundance spans 3 orders of magnitude and increases in the following order: marine aerosols; continental aerosols; and, finally, dust plumes. Biological particles are important INPs observed in continental and marine aerosols, whereas they play a secondary, although important, role during Saharan dust events. Air masses in the planetary boundary layer (PBL) show both enriched INP concentrations and a higher proportion of INPs to total aerosol particles, compared with cases in the FT. The presence of precipitation/clouds enriches INPs in the FT but decreases INPs in the PBL. Additionally, new INP parameterizations are developed that incorporate the ratio of fluorescent-to-nonfluorescent or coarse-to-fine particles and predict >90 % of the observed INPs within an uncertainty range of a factor of 10; these new parameterizations exhibit better performance than current widely used parameterizations and allow ice formation in models to respond to variations in dust and biological particles. The improved parameterizations can help MPC formation simulations in regions with various INP sources or different regions with prevailing INP sources.

Influence of columnar versus vertical distribution of aerosol properties on the modulation of shortwave radiative effects

Quantifying the interaction of atmospheric aerosols with incoming solar radiation remains a challenge owing to the limitations associated with measuring aerosol optical properties. This study investigates how the distribution of aerosol properties, whether columnar or vertical, affects the aerosol radiative forcing (ARF) and heating rates (HRs) across different atmospheric layers under cloud-free conditions in the shortwave region. We also assess the atmospheric parameters, namely, pressure, temperature, water vapour density, and ozone density, from in-situ measurements, reanalysis data, and a standard tropical atmosphere to understand their impact on ARF and HR estimates across seasons. Our findings show that aerosol absorption is highest during monsoon, while it is lowest in the winter. Significant atmospheric warming due to aerosols resulted from the substantial cooling at the surface. Columnar properties of aerosols measured at limited or multiple wavelengths yield similar ARF and HR estimates, provided spectral dependency is considered using the Angstrom exponent across seasons. However, the vertical profiles of aerosol extinction, together with a constant single scattering albedo (SSA) along the atmospheric column versus an actual SSA profile, led to notable differences in ARF and HRs, specifically in pre-monsoon and monsoon periods. Free tropospheric aerosol absorption is underestimated when using columnar properties compared to vertical distribution, while boundary layer absorption is overestimated (> 10 Wm-2). The heterogeneity in aerosol types across atmospheric layers significantly influenced aerosol absorption, highlighting the importance of accurate vertical distribution information. HR profiles obtained with vertical distribution reflect the structure of aerosol extinction, whereas those estimated with columnar properties result in smoother profiles that fail to capture altitude gradients. Aerosol-induced HRs are higher within the boundary layer and free troposphere in the monsoon season for all scenarios of defined aerosol properties. These findings underscore the need for actual vertical profile measurements of aerosol properties to quantify aerosol radiation interaction.

Tropical tropospheric ozone distribution and trends from in situ and satellite data

Abstract. Tropical tropospheric ozone (TTO) is important for the global radiation budget because the longwave radiative effect of tropospheric ozone is higher in the tropics than midlatitudes. In recent decades the TTO burden has increased, partly due to the ongoing shift of ozone precursor emissions from midlatitude regions toward the Equator. In this study, we assess the distribution and trends of TTO using ozone profiles measured by high-quality in situ instruments from the IAGOS (In-Service Aircraft for a Global Observing System) commercial aircraft, the SHADOZ (Southern Hemisphere ADditional OZonesondes) network, and the ATom (Atmospheric Tomographic Mission) aircraft campaign, as well as six satellite records reporting tropical tropospheric column ozone (TTCO): TROPOspheric Monitoring Instrument (TROPOMI), Ozone Monitoring Instrument (OMI), OMI/Microwave Limb Sounder (MLS), Ozone Mapping Profiler Suite (OMPS)/Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2), Cross-track Infrared Sounder (CrIS), and Infrared Atmospheric Sounding Interferometer (IASI)/Global Ozone Monitoring Experiment 2 (GOME2). With greater availability of ozone profiles across the tropics we can now demonstrate that tropical India is among the most polluted regions (e.g., western Africa, tropical South Atlantic, Southeast Asia, Malaysia and Indonesia), with present-day 95th percentile ozone values reaching 80 nmol mol−1 in the lower free troposphere, comparable to midlatitude regions such as northeastern China and Korea. In situ observations show that TTO increased between 1994 and 2019, with the largest mid- and upper-tropospheric increases above India, Southeast Asia, and Malaysia and Indonesia (from 3.4 ± 0.8 to 6.8 ± 1.8 nmol mol−1 decade−1), reaching 11 ± 2.4 and 8 ± 0.8 nmol mol−1 decade−1 close to the surface (India and Malaysia–Indonesia, respectively). The longest continuous satellite records only span 2004–2019 but also show increasing ozone across the tropics when their full sampling is considered, with maximum trends over Southeast Asia of 2.31 ± 1.34 nmol mol−1 decade−1 (OMI) and 1.69 ± 0.89 nmol mol−1 decade−1 (OMI/MLS). In general, the sparsely sampled aircraft and ozonesonde records do not detect the 2004–2019 ozone increase, which could be due to the genuine trends on this timescale being masked by the additional uncertainty resulting from sparse sampling. The fact that the sign of the trends detected with satellite records changes above three IAGOS regions, when their sampling frequency is limited to that of the in situ observations, demonstrates the limitations of sparse in situ sampling strategies. This study exposes the need to maintain and develop high-frequency continuous observations (in situ and remote sensing) above the tropical Pacific Ocean, the Indian Ocean, western Africa, and South Asia in order to estimate accurate and precise ozone trends for these regions. In contrast, Southeast Asia and Malaysia–Indonesia are regions with such strong increases in ozone that the current in situ sampling frequency is adequate to detect the trends on a relatively short 15-year timescale.

Elevated Tropospheric Iodine Over the Central Continental United States: Is Iodine a Major Oxidant of Atmospheric Mercury?

AbstractPrevious efforts to measure atmospheric iodine have focused on marine and coastal regions. We report the first ground‐based tropospheric iodine monoxide (IO) radical observations over the central continental United States. Throughout April 2022, IO columns above Storm Peak Laboratory, Colorado (3,220 m.a.s.l.) ranged from 0.7 ± 0.5 to 3.6 ± 0.5 × 1012 (average: 1.9 × 1012 molec cm−2). IO was consistently elevated in air masses transported from over the Pacific Ocean. The observed IO columns were up to three times higher and the range was larger than predicted by a global model, which warrants further investigation into iodine sources, sinks, ozone loss, and particle formation. IO mixing ratios increased with altitude. At the observed levels, iodine may be competitive with bromine as an oxidant of elemental mercury at cold temperatures typical of the free troposphere. Iodine‐induced mercury oxidation is missing in atmospheric models, understudied, and helps explain model underestimation of oxidized mercury measurements.

Precursor boundary layer conditions for shallow and deep convection: inferences from CAIPEEX field measurements over the Indian Peninsula

The diurnal cycle of environmental conditions for shallow and deep convection regimes within the Indian monsoon environment is investigated using comprehensive observations from the surface, boundary layer, and cloud layers. For shallow convection (SC) and deep convection (DC) in the afternoon hours, thermodynamics, moisture convergence, and several other environmental variables provide information on the factors that control the vertical extent of convection in both regimes. The SC regime is characterized by high sensible heat flux, leading to stronger boundary layer turbulence, a higher mixed layer, and increased dry air entrainment from the free troposphere. Evaluation of several pre-conditioning parameters with T-test statistics suggests that stronger mid-level meridional wind shear and lack of mid-level moistening are detrimental to the growth of clouds in the SC regime. Conversely, the DC regime is driven by low surface fluxes and low surface-level buoyancy, with higher boundary layer and mid-layer moisture and more mid-layer instability, supporting larger Convective Available Potential Energy (CAPE). Morning precursor conditions for the preference of SC versus DC regime in the afternoon reveal that total column water vapor, relative humidity and CAPE are significantly higher on DC days. Large-scale moisture transport in the early morning within and above the boundary layer, driven by stronger westerly winds, is a key factor for the development of DC later in the day. This investigation enhances our understanding of boundary layer controls on shallow and deep convection within the Indian Monsoon environment.

AN ANALYSIS OF WIND SPEED VARIATIONS INSIDE AND OUTSIDE OF THE ATMOSPHERIC BOUNDARY LAYER DURING CONVECTIVE STORMS USING SODAR AND RADIOSONDE DATA

This paper analyzes the mean wind speed variations inside the atmospheric boundary layer and in the free troposphere based on data from vertical sounding of the atmosphere using SODAR and radiosonde data. The variation of the mean wind speed inside and outside of the atmospheric boundary layer were analyzed using data collected during warnings of convective storms, but also 12 hours before and after the alerts. The resulting data are important in understanding the way the wind behaves in the atmospheric boundary layer and the free troposphere before, during and after convective events.

Vapor-Buoyancy Feedback in an Idealized GCM

Abstract Humid air is lighter than dry air at a given temperature and pressure, as the molecular weight of water vapor is less than that of dry air. This effect is known as vapor buoyancy (VB). Although this effect is a well-understood consequence of the ideal gas law, its influence on climate has been under-studied. This study investigates VB’s influence on atmospheric temperature, radiation, and clouds. In mechanism-denial experiments, we remove VB from the dynamics and parameterizations of an idealized general circulation model (GCM). These experiments show that VB warms the tropical free troposphere by approximately 1 K in an Earth-like climate, and the magnitude of this effect increases with warming. This additional atmospheric warming causes greater outgoing longwave radiation (OLR) to be emitted as the climate warms. This constitutes a negative climate feedback which attains a magnitude of 0.1 to 0.2 W/m2/K in the tropics. The simulations further show that, despite warming the atmosphere, VB does not introduce a countervailing positive water vapor feedback. Finally, we find that VB makes the net cloud feedback in the model more negative than it otherwise would be, reinforcing the clear-sky feedback.

Identification of organic constituents on atmospheric particulate matter in the East Asian background air of free troposphere by GC×GC-TOFMS

The presence of organic compounds on the particulate matter (PM) or aerosols can arise from the condensation of gaseous organic compounds on the existing aerosols, or from organic precursors to form secondary organic aerosols (SOA) through photochemistry. The objective of this study is to characterize organic constituents on aerosols relevant to their emission sources and the key compounds revealing the evolution of aerosols with the use of a novel analytical technique. A time-of-flight mass spectrometry (TOFMS) coupled with comprehensive two-dimensional gas chromatography (GC×GC) was developed using a flow type of modulator instead of a thermal type as a prelude to field applications without the need for cryogen. The methodology of GC×GC-TOFMS is discussed in this study in detail.Since the coarse PM (PM10-2.5) may exhibit with a relatively high OC content compared to PM2.5, the GC×GC results have been obtained by analyzing PM10 samples collected in parallel with OC/EC analysis of PM2.5 samples at the Lulin Atmospheric Background Station (LABS, 23.47°N, 120.87°E, 2862 m ASL) as the high-mountain background site in East Asia. We found that the organic analytes were in a majority in the range of 12–30 carbon numbers falling in the category of semi-volatile organic compounds (SVOCs) with 43 compounds of alcohol, aldehyde, ketone, and ester varieties if excluding alkanes. Intriguingly, trace amounts of plasticizers and phosphorus flame retardants such as phthalates (PAEs) and triphenyl phosphate (TPP) were also found, likely originating from regions involved in open burning of household solid waste in Southeast Asia or e-waste recycling in southern China and along the long-range transport route. Compounds such as these are unique to the specific sources, demonstrating the wide spread of these hazardous compounds in the environment.

Impacts of free tropospheric turbulence parametrisation on a sheared tropical cyclone

AbstractThe turbulent transport of momentum, heat, and moisture can impact tropical cyclone intensity. However, representing subgrid‐scale turbulence accurately in numerical weather prediction models is challenging due to a lack of observational data. To address this issue, a case study of Hurricane Maria was conducted to analyse the influence of different free tropospheric turbulence parametrisations on sheared tropical cyclones. The study used the current Met Office Unified Model (MetUM) parametrisation, as well as a parametrisation scheme with significantly reduced free tropospheric mixing length. Convection‐permitting ensemble simulations were performed for both mixing schemes at two initialisation times (four 18‐member ensembles in total), revealing an improvement in the intensity forecasts of Hurricane Maria when the mixing length was decreased in the free troposphere. By implementing this change, the less diffuse simulations presented a drier mid‐level. The resolved downward transport of drier air from the mid‐levels into the inflow layer (so‐called “downdraft ventilation”) was thus more effective in reducing the storm's intensity. In contrast to earlier studies, where decreasing the diffusivity in the boundary layer intensified the storm, we show that decreasing the free tropospheric diffusivity can weaken the storm by enhancing shear‐related weakening processes. While this study was performed using the MetUM, the findings highlight the general importance of considering turbulence parametrisation, and show that changes in diffusivity can have different impacts on storm intensity depending on the environment and where the changes are applied.

Elucidating the boundary layer turbulence dissipation rate using high-resolution measurements from a radar wind profiler network over the Tibetan Plateau

Abstract. The planetary boundary layer (PBL) over the Tibetan Plateau (TP) exerts a significant influence on regional and global climate, while its vertical structures of turbulence and evolution features remain poorly understood, largely due to the scarcity of observations. This study examines the vertical profile of and daytime variation in the turbulence dissipation rate (ε) in the PBL and free troposphere over the TP using the high-resolution (6 min and 120 m) measurements from a radar wind profiler (RWP) network, combined with hourly data from ERA5 during the period from 1 September 2022 to 31 October 2023. Observational analyses show that the magnitude of ε below 3 km under all-sky conditions exhibits a large spatial discrepancy over the six RWP stations over the TP. Particularly, the values of ε at Minfeng and Jiuquan over the northern TP and at Dingri (alternately Tingri) over the southern TP are roughly an order of magnitude greater than those at Lijiang, Ganzi (alternately Garzê), and Hongyuan over the eastern TP. This could be partially attributed to the difference in land cover across the six RWP stations. In terms of the diurnal variation, ε rapidly intensifies from 09:00 local standard time (LST) to 14:00 LST and then gradually levels off in the late afternoon. Under clear-sky conditions, both ε and the planetary boundary layer height (zi) are greater compared with cloudy-sky conditions, which could be due to the cooling effect of clouds, which reduces the solar irradiation reaching the surface. In the lower PBL (0.3 ≤ z/zi ≤ 0.5), where z is the height above ground level, the dominant influential factor in the development of turbulence is the surface–air temperature difference (Ts−Ta). By comparison, in the upper PBL (0.6 ≤ z/zi ≤ 1.0), both Ts−Ta and vertical wind shear (VWS) affect the development of turbulence. Above the PBL (1.0 < z/zi ≤ 2.0), the shear production resulting from VWS dominates the variation in turbulence. Under cloudy-sky conditions, the reduced Ts−Ta and weakened surface sensible heat flux tend to inhibit the turbulent motion in the PBL. On the other hand, the strong VWS induced by clouds enhances the turbulence above the PBL. The findings obtained here underscore the importance of the RWP network in revealing the fine-scale structures of the PBL over the TP and gaining new insight into the PBL evolution.