Trace Gas Species Research Articles

Synthesizing gas-filled anti-resonant hollow-core fiber Raman lines enables access to the molecular fingerprint region

The synthesis of multiple narrow optical spectral lines, precisely and independently tuned across the near- to mid-infrared region, is a pivotal research area that enables selective and real-time detection of trace gas species within complex gas mixtures. However, existing methods for developing such light sources suffer from limited flexibility and very low pulse energy, particularly in the mid-infrared domain. Here, we introduce a concept that is based on the combination of an appropriate design of near-infrared fiber laser pump and cascaded configuration of gas-filled anti-resonant hollow-core fiber technology. This concept enables the synthesis of multiple independently tunable spectral lines, with >1 μJ high pulse energies and a few nanoseconds pulse width in the near- and mid-infrared regions. The number and wavelengths of the generated spectral lines can be dynamically reconfigured. A proof-of-concept laser beam synthesized of two narrow spectral lines at 3.99 µm and 4.25 µm wavelengths is demonstrated and combined with photoacoustic modality for real-time SO2 and CO2 detection. The proposed concept also constitutes a promising way for infrared multispectral microscopic imaging.

Planetary Waves Drive Horizontal Variations in Trace Species in the Venus Deep Atmosphere

Abstract The deep atmosphere of Venus remains mysterious because of the planet’s high, optically thick cloud decks. While phenomena such as the observed decadal fluctuations in sulfur dioxide abundance above the clouds could shed light on conditions below, poor understanding of vertical and horizontal transport limits such an approach. Nightside spectral windows permit observation of trace gas species in the lower atmosphere, but incomplete understanding of the circulation makes the distribution of these species challenging to interpret. We performed two simulations with the Venus Planetary Climate Model including an age of air calculation to investigate tracer transport (a) between the surface and the stagnant lower haze layer and (b) between the cloud deck and the observable upper atmosphere. We find a timescale on the order of many decades for surface-to-lower haze layer transport and ∼1.4 yr from the lowest cloud deck to 101 km. The extreme slowness of transport from the surface to the clouds makes it unlikely that compositional variability at the surface could affect the upper atmosphere sulfur dioxide abundance on observed timescales. Planetary-scale Rossby waves with a zonal wavenumber of 1 in both hemispheres are found to circumnavigate the planet in the deep atmosphere in 36 Earth days. These waves are associated with gyres that collect tracers and areas of upwelling that transport them to higher altitudes, leading to significantly younger air at polar latitudes in the altitude range of 25–45 km. The existence of chemically enhanced traveling Rossby gyres could explain the observed deep atmosphere carbon monoxide variability.

Water vapor condensation in optical instruments on Mars

Modern high-sensitivity spectrometers rely on photons reflecting thousands of times between extremely reflective mirrors to generate absorption pathlengths that are kilometers long. The absorption spectrum of trace gas species is enhanced when cooling the gas sample, however, should any atmospheric volatiles condense within the gas cell, the highly-reflective mirrors may become marred, drastically cutting down the effective optical path length. In the Martian atmosphere, the first volatile to condense is typically water vapor, thus understanding the variability of the water frost point is essential for determining the performance limit of any optical instrument. We will examine these performance limits and map the maximum temperatures at which water vapor will condense on the Martian surface with respect to a model instrument being prepared for flight. The variability of the frost point with time and solar longitude (Ls) therefore reveals areas of the Martian surface at which the precision of a high-sensitivity spectrometer is optimized. We find that the optimal performance is achieved during northern fall and winter (Ls = 180°–360°) at polar and mid-latitude locations in the northern hemisphere, and during northern spring (Ls = 0°–90°) at equatorial and mid-latitude locations in the southern hemisphere when the frost point reaches the lowest maximums.

A mini broadband cavity enhanced absorption spectrometer for nitrogen dioxide measurement on the unmanned aerial vehicle platform

We developed a small size and light weight analyzer based on the broadband cavity enhanced absorption spectroscopy for measuring nitrogen dioxide (NO2) with high spatial-temporal resolution and high accuracy. The instrument utilizes a LED centered at 450 nm, a short optical cavity, and a spectrometer to determine the extinction coefficients span 435–465 nm, allowing us to retrieve the mixing ratio of NO2 by absorption cross-section. The measurement precision (1σ) for NO2 is 98 ppt in 2 s under laboratory conditions. The uncertainty is estimated at 6% mainly attributed to cross-section and the mirror reflectivity. Good consistency was achieved by comparing with commercial chemiluminescence detector and cavity attenuation phase shift spectrometer (CAPS) (both R2 = 0.99). We further mounted the instrument on an unmanned aerial vehicle (UAV), and maintained the UAV flight at the height of 20 m, the comparative measurement with a CAPS set in a neighbor building with the same sampling height showed a good correlation (R2 = 0.97), which confirmed the instrumental feasibility and stability on the UAV platform. At last, we present a successful NO2 vertical measurement test, the good performance indicates this portable technique has great potential for vertical measurement. In particular, the mini-CEAS technique can further extend to measure the vertical profiles of other trace gas species (such as nitrous acid) with strong optical structural absorptions, which would largely promote the understanding of atmospheric chemistry on a vertical scale.

Iron-sulfur chemistry can explain the ultraviolet absorber in the clouds of Venus.

The clouds of Venus are believed to be composed of sulfuric acid (H2SO4) and minor constituents including iron-bearing compounds, and their respective concentrations vary with height in the thick Venusian atmosphere. This study experimentally investigates possible iron-bearing mineral phases that are stable under the unique conditions within Venusian clouds. Our results demonstrate that ferric iron can react with sulfuric acid to form two mineral phases: rhomboclase [(H5O2)Fe(SO4)2·3H2O] and acid ferric sulfate [(H3O)Fe(SO4)2]. A combination of these two mineral phases and dissolved Fe3+ in varying concentrations of sulfuric acid are shown to be good candidates for explaining the 200- to 300-nm and 300- to 500-nm features of the reported unknown UV absorber. We, therefore, hypothesize a rich and largely unexplored heterogeneous chemistry in the cloud droplets of Venus that has a large effect on the optical properties of the clouds and the behavior of trace gas species throughout Venus's atmosphere.

Stability Characterisation and Application of Mutually Injection Locked Gain Switched Optical Frequency Combs for Dual Comb Spectroscopy

The application of two gain switched optical frequency combs (OFCs) in dual comb gas phase spectroscopy is demonstrated. We report on the stability analysis of the wavelength and power of individual comb lines of the two OFCs. The examination reveals that a maximum wavelength fluctuation of <2.5 pm and a maximum peak power fluctuation of ∼0.3 dB is achievable for the OFCs. The radio frequency (RF) beat tone spectrum shows the standard deviation of the peak power of an individual beat tone from the mean is as low as ∼0.14 dB with negligible frequency fluctuations. In a proof-of-principle experiment the dual comb system is applied to the detection of hydrogen sulphide (H2S) with a detection sensitivity of (740 ± 160) ppmv, demonstrating its excellent frequency and power stability. The dual OFCs can in principle be monolithically integrated and thus enable the development of compact, cost-efficient dual comb devices, for the detection of multiple trace gas species or isotopologues.

An extensive database of airborne trace gas and meteorological observations from the Alpha Jet Atmospheric eXperiment (AJAX)

Abstract. The Alpha Jet Atmospheric eXperiment (AJAX) flew scientific flights between 2011 and 2018 providing measurements of trace gas species and meteorological parameters over California and Nevada, USA. This paper describes the observations made by the AJAX program over 229 flights and approximately 450 h of flying. AJAX was a multi-year, multi-objective, multi-instrument program with a variety of sampling strategies resulting in an extensive dataset of interest to a wide variety of users. Some of the more common flight objectives include satellite calibration/validation (GOSAT, OCO-2, TROPOMI) at Railroad Valley and other locations and long-term observations of free-tropospheric and boundary layer ozone allowing for studies of stratosphere-to-troposphere transport and long-range transport to the western United States. AJAX also performed topical studies such as sampling wildfire emissions, urban outflow and atmospheric rivers. Airborne measurements of carbon dioxide, methane, ozone, formaldehyde, water vapor, temperature, pressure and 3-D winds made by the AJAX program have been published at NASA's Airborne Science Data Center (https://asdc.larc.nasa.gov/project/AJAXTS9 (last access: 1 November 2022), https://doi.org/10.5067/ASDC/SUBORBITAL/AJAX/DATA001, Iraci et al., 2021a).

Mean age from observations in the lowermost stratosphere: an improved method and interhemispheric differences

Abstract. The age of stratospheric air is a concept commonly used to evaluate transport timescales in atmospheric models. The mean age can be derived from observations of a single long-lived trace gas species with a known tropospheric trend. Commonly, deriving mean age is based on the assumption that all air enters the stratosphere through the tropical (TR) tropopause. However, in the lowermost stratosphere (LMS) close to the extra-tropical (exTR) tropopause, cross-tropopause transport needs to be taken into account. We introduce the new exTR–TR method, which considers exTR input into the stratosphere in addition to TR input. We apply the exTR–TR method to in situ SF6 measurements from three aircraft campaigns (PGS, WISE and SouthTRAC) and compare results to those from the conventional TR-only method. Using the TR-only method, negative mean age values are derived in the LMS close to the tropopause during the WISE campaign in Northern Hemispheric (NH) fall 2017. Using the new exTR–TR method instead, the number and extent of negative mean age values is reduced. With our new exTR–TR method, we are thus able to derive more realistic values of typical transport times in the LMS from in situ SF6 measurements. Absolute differences between both methods range from 0.3 to 0.4 years among the three campaigns. Interhemispheric differences in mean age are found when comparing seasonally overlapping campaign phases from the PGS and the SouthTRAC campaigns. On average, within the lowest 65 K potential temperature above the tropopause, the NH LMS is 0.5±0.3 years older around March 2016 than the Southern Hemispheric (SH) LMS around September 2019. The derived differences between results from the exTR–TR method and the TR-only method, as well as interhemispheric differences, are higher than the sensitivities of the exTR–TR method to parameter uncertainties, which are estimated to be below 0.22 years for all three campaigns.

Numerical study of transverse jet mixing and combustion in a high-enthalpy supersonic crossflow with trace gases

High-enthalpy gas streams in a real engine or wind tunnel will contain some trace gases; however, this is often ignored in many studies. To investigate transverse fuel-jet mixing and combustion characteristics in a high-enthalpy inflow with trace-gas species, large-eddy simulations based on the HyShot II configuration have been adopted and verified. It was found that a trace amount of atomic oxygen (O) and nitrous oxide has a direct significance on ignition delay times and can, therefore, influence the overall flame distribution. In addition, the results show a greater sensitivity to the levels of O. The complex shock-wave system generated by the transverse jet is found to be a key factor in enhancing mixing and inducing combustion. It not only facilitates vortex generation by increasing the baroclinic term but also provides regions with high pressure and temperature, which accelerate the chemical-reaction rates for radical generation. The initial ignition locations, characterized by HO2 production rates, are mainly located in the low-speed region close to the injector, e.g., in the recirculation region, while OH is mainly formed downstream and accompanied by strong heat release. Based on the analysis of instantaneous contours and statistical results, the overall combustion was found to be in scramjet mode. The partially premixed flame dominates the combustor, where the combustion mainly lies in the flamelet regime, while the diffusion flame dominates the nozzle, where the combustion is spread over the flamelet regime, the broken flamelet regime, and the perfectly stirred reactor regime.

Evaluating the Value of CrIS Shortwave-Infrared Channels in Atmospheric-Sounding Retrievals

The Cross-track Infrared Sounder (CrIS), in low Earth orbit since 2011, makes measurements of the top of atmosphere radiance for input into data assimilation (DA) systems as well as the retrieval of geophysical state variables. CrIS measurements have 2211 narrow infrared channels ranging between 650 and 2550 cm−1 (~3.9–15.4 μm) and capture the variation in profiles of atmospheric temperature, water vapor, and numerous trace gas species. DA systems derive atmospheric temperature by assimilating CO2-sensitive channels in the CrIS longwave (LW) band (650–1095 cm−1). Here, we investigate if CO2-sensitive channels in the shortwave (SW) band (2155–2550 cm−1) can similarly be applied. We first evaluated the information content of the CrIS bands followed by an assessment of the performance degradation of retrievals due to the loss of individual CrIS bands. We found that temperature profile retrievals derived from the CrIS SW band were statistically both well-behaved and as accurate as a retrieval utilizing the CrIS LW band. The one caveat, however, is that the higher CrIS instrument noise in the SW band limited its performance under certain conditions. We conclude with a discussion on the implications our results have for channel selection in retrieval and DA systems as well as the design of future space instruments.

Design of an array structure for carbon-based field-effect-transistor type gas sensors to accurately identify trace gas species

A carbon-based FET gas sensor with a noble metal nanoparticles/Co3O4 composites sensing gate is proposed to detect trace gases as low to 80 ppb. A sensor array with different sensing gates is designed to achieve accurate recognition of gases.

Cavity ring-down spectroscopy of water vapor in the deep-blue region

Abstract. Water vapor absorption in the near-ultraviolet region is essential to describe the energy budget of Earth, but little spectroscopic information is available since it is a challenging spectral region for both experimental and theoretical studies. A continuous-wave cavity ring-down spectroscopic experiment was built to record absorption lines of water vapor around 415 nm. With a precision of 4×10-10 cm−1, 40 rovibrational transitions of H216O were observed in this work, and 27 of them were assigned to the (224), (205), (710), (304), (093), (125) and (531) vibrational bands. A comparison of line positions and intensities determined in this work to the most recent HITRAN database is presented. Water vapor absorption cross-sections near 415 nm were calculated based on our measurements, which vary between 1×10-26 and 5×10-26cm2 molec.−1. These data will also significantly impact the spectroscopy detection of trace gas species in the near-UV region.

Assessing JUICE's ability of in situ plume detection in Europa's atmosphere

ESA's upcoming JUpiter Icy moons Explorer (JUICE) is scheduled to perform two flybys of Jupiter's moon Europa. Here, we present the results of our investigation into JUICE's capability to detect plumes and to separate them from the background water in the atmosphere as a function of their source's location and mass flux on the Europan surface using the neutral mass spectrometer NIM. For both of the currently planned flybys we evaluate different scenarios to estimate how feasible such a detection is, using a Monte Carlo particle tracing model of a plume. We also incorporate the putative plume candidates reported by Roth et al. (2014b), Sparks et al. (2016), Sparks et al. (2017), Jia et al. (2018), Arnold et al. (2019) and Sparks et al. (2019) into this investigation. We come to the conclusion that the first flyby trajectory is better suited to detect the potential plume candidates listed above as they are detectable down to mass fluxes of approx. 100 ​kg/s. The second flyby requires mass fluxes between 100 ​kg/s and 500 ​kg/s for all suggested plume candidates to be detectable. This discrepancy is caused by the first flyby's closer proximity to the locations of the suggested plume sources which lie mainly on the southern hemisphere. Separation of water plumes from the atmospheric water vapour density is dependent on the mass flux of the respective plume source. The only plume separable from the background water in the atmosphere at the lowest investigated plume source mass flux of 1 ​kg/s is the one suggested by Roth et al. (2014b). It is therefore the most likely plume to be detected by JUICE. Furthermore, we investigate the detectability of trace gas contents in a plume and analyse how these impact upon plume detection. The spacecraft will be able to detect whether lighter-than-water trace gas species are present within the plume down to trace gas source mass fluxes of 0.1 ​kg/s. Provided this is the case, such species constitute a means to identifying plumes in the Europan atmosphere. Finally, the effects of lowering the flyby altitude are examined. We find that lowering the altitude of the CA does not increase the region of separability. Therefore, lowering the second flyby trajectory will not suffice for the spacecraft to be able to identify plumes that originate from the locations of the candidates mentioned above. Considering that the second flyby is the most likely to be lowered, this case study provides an example of the importance of arranging the second trajectory in a manner such that its ground track lies in close proximity to the locations of the suggested plume candidates listed above. This approach to the mission planning maximises the chance of separating the presumptive plumes from the atmospheric background water even at the lowest plume source mass fluxes.

Phase-wise analysis of the COVID-19 lockdown impact on aerosol, radiation and trace gases and associated chemistry in a tropical rural environment

Phase-wise variations in different aerosol (BC, AOD, PM1, PM2.5 and PM10), radiation (direct and diffused) and trace gases (NO, NO2, CO, O3, SO2, CO2 and CH4) and their associated chemistry during the COVID-19 lockdown have been investigated over a tropical rural site Gadanki (13.5° N, 79.2° E), India. Unlike most of the other reported studies on COVID-19 lockdown, this study provides variations over a unique tropical rural environment located at a scientifically strategic location in the Southern Indian peninsula. Striking differences in the time series and diurnal variability have been observed in different phases of the lockdown. The levels of most species that are primarily emitted from anthropogenic activities reduced significantly during the lockdown which also impacted the levels and diurnal variability of secondary species like O3. When compared with the same periods in 2019, short-lived trace gas species such as NO, NO2, SO2 which have direct anthropogenic emission influence have shown the reduction over 50%, whereas species like CO and O3 which have direct as well as indirect impacts of anthropogenic emissions have shown reductions up to 10%. Long-lived species (CO2 and CH4) have shown negligible difference (<1%). BC and AOD have shown reductions over 20%. Particulate Matter (1, 2.5 and 10) reductions have been in the range of 40 to 50% when compared to the pre-lockdown period. The changes in shortwave downward radiation at the surface, diffuse component due to the scattering and diffuse fraction have been +2.2%, −4.1% and −2.4%, respectively, in comparison with 2019. In contrast with the studies over urban environments, air quality category over the rural environment remained same during the lockdown despite reduction in pollutants level. All the variations observed for different species and their associated chemistry provides an excellent demonstration of rural atmospheric chemistry and its intrinsic links with the precursor concentrations and dynamics.

Measurement report: Aircraft observations of ozone, nitrogen oxides, and volatile organic compounds over Hebei Province, China

Abstract. To provide insight into the planetary boundary layer (PBL) production of ozone (O3) over the North China Plain, the Air chemistry Research in Asia (ARIAs) campaign conducted aircraft measurements of air pollutants over Hebei Province, China, between May and June 2016. We evaluate vertical profiles of trace gas species including O3, nitrogen oxides (NOx), carbon monoxide (CO), and volatile organic compounds (VOCs) and relate to rates of O3 production. This analysis shows measured O3 levels ranged from 45 to 146 ppbv, with the peak median concentration (∼ 92 ppbv) occurring between 1000 and 1500 m. The NOx concentrations exhibited strong spatial and altitudinal variations, with a maximum of 53 ppbv. Ratios of CO∕CO2 indicate the prevalence of low-efficiency combustion from biomass burning and residential coal burning but indicate some success of regional pollution controls compared to earlier studies in China. Concentrations of total measured VOCs reveal alkanes dominate the total measured volume mixing ratio of VOCs (68 %), and sources include vehicular emissions, fuel and solvent evaporation, and biomass burning. Alkanes and alkenes/alkynes are responsible for 74 % of the total VOC reactivity assessed by calculating the OH loss rates, while aromatics contribute the most to the total ozone formation potential (OFP) (43 %) with toluene, m/p-xylene, ethylene, propylene, and i-pentane playing significant roles in the aloft production of O3 in this region. In the PBL below 500 m, box model calculations constrained by measured precursors indicate the peak rate of mean O3 production was ∼ 7 ppbv h−1. Pollution frequently extended above the PBL into the lower free troposphere around 3000 m, where NO2 mixing ratios (∼ 400 pptv) led to net production rates of O3 up to ∼ 3 ppbv h−1; this pollution can travel substantial distances downwind. The O3 sensitivity regime is determined to be NOx-limited throughout the PBL, whereas it is more VOC-limited at low altitudes near urban centers, demonstrating that control of both VOCs and NOx is needed to reduce aloft O3 pollution over Hebei.

On deriving influences of upwind agricultural and anthropogenic emissions on greenhouse gas concentrations and air quality over Delhi in India: A stochastic Lagrangian footprint approach

Delhi, the capital city of India witnesses severe degradation of air quality and rapid enhancement of trace gases during winter. Still it is unclear about the relative role of the meteorological conditions and the post-monsoon agricultural stubble burning on the occurrence of these events. To overcome this, we examine the use of applying high-resolution transport model to establish the link between atmospheric concentrations and upstream surface fluxes. This study reports the implementation of a Lagrangian approach and demonstrates its capability in deriving the upwind influences over Delhi. We simulate stochastic back trajectories over Delhi by implementing stochastic time-inverted Lagrangian transport (STILT) model, driven by the meteorological fields from the European Centre for Medium Range Weather Forecasts (ECMWF) model. During the post-monsoon, when mixing layer height is shallow, we find high near-field influence. The variations in footprint simulations with receptor heights show the effect of mixing layer dynamics on the air-parcels. By using atemporal emission fields, we find a considerable impact of meteorological conditions during November that contributes to the enhancements of trace gases. Together with strong emissions (anthropogenic and biomass burning), these enhancements can be several orders higher compared to other seasons. Through the receptor-oriented STILT implementation over India, we envision a wide range of applications spanning from air quality to climate change. An advantage of this implementation is that it allows the use of pre-calculated footprints in simulating any trace gas species and particulate matter, making it computationally less demanding than running an ensemble of full atmospheric transport model.

Potential vorticity structure of Titan’s polar vortices from Cassini CIRS observations

The Cassini mission has provided the best opportunity to date to extensively study the seasonal variation in Titan’s atmosphere, with observations spanning almost half a Titan year (Ls=293−93°). An important feature in the Titan middle-atmosphere is the formation of a polar vortex. Observations have shown that an initially well-developed northern vortex enriched with trace gas species gradually breaks down after spring equinox as a new vortex emerges in southern winter. Here we use Cassini CIRS observations to derive the temperature and composition of the middle-atmosphere. We use the gradient wind equation to first estimate the mean zonal winds, and then the Potential Vorticity (PV) throughout Titan’s atmosphere over the timespan of the Cassini mission. PV is a useful diagnostic quantity for studying the dynamics of polar vortices because it is materially conserved for adiabatic and frictionless flows, and can be inverted to find all other dynamical fields. Our results show the formation of a strong zonal jet in the winter hemisphere, with wind velocities reaching 220 ms−1, which is consistent with previous studies. An annular PV structure is also observed over the winter poles, whereby a ring of PV encircles a local minima over the pole. Such distributions are often found to be unstable without a restoring force, yet they are seen here in numerous observations in both the northern and southern hemispheres. A comparison with the annular Martian vortices shows that latent heat release from condensation or subsidence-induced adiabatic heating may explain the origin and stability of the annulus. Finally, we investigate the evolution of the size of the vortices and the role of strong PV gradients as a dynamical mixing barrier for trace gas species across the vortex edge. We find that longer lived gases are less confined to the vortex than those with shorter photochemical lifetimes.

Evaluation of a field-deployable Nafion™-based air-drying system for collecting whole air samples and its application to stable isotope measurements of CO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;

Abstract. Atmospheric flask samples are either collected at atmospheric pressure by opening a valve of a pre-evacuated flask or pressurized with the help of a pump to a few bar above ambient pressure. Under humid conditions, there is a risk that water vapor in the sample leads to condensation on the walls of the flask, notably at higher than ambient sampling pressures. Liquid water in sample flasks is known to affect the CO2 mixing ratios and also alters the isotopic composition of oxygen (17O and 18O) in CO2 via isotopic equilibration. Hence, for accurate determination of CO2 mole fractions and its stable isotopic composition, it is vital to dry the air samples to a sufficiently low dew point before they are pressurized in flasks to avoid condensation. Moreover, the drying system itself should not influence the mixing ratio and the isotopic composition of CO2 or that of the other constituents under study. For the Airborne Stable Isotopes of Carbon from the Amazon (ASICA) project focusing on accurate measurements of CO2 and its singly substituted stable isotopologues over the Amazon, an air-drying system capable of removing water vapor from air sampled at a dew point lower than −2 ∘C, flow rates up to 12 L min−1 and without the need for electrical power was needed. Since to date no commercial air-drying device that meets these requirements has been available, we designed and built our own consumable-free, power-free and portable drying system based on multitube Nafion™ gas sample driers (Perma Pure, Lakewood, USA). The required dry purge air is provided by feeding the exhaust flow of the flask sampling system through a dry molecular sieve (type 3A) cartridge. In this study we describe the systematic evaluation of our Nafion™-based air sample dryer with emphasis on its performance concerning the measurements of atmospheric CO2 mole fractions and the three singly substituted isotopologues of CO2 (16O13C16O, 16O12C17O and 16O12C18O), as well as the trace gas species CH4, CO, N2O and SF6. Experimental results simulating extreme tropical conditions (saturated air at 33 ∘C) indicated that the response of the air dryer is almost instantaneous and that approximately 85 L of air, containing up to 4 % water vapor, can be processed staying below a −2 ∘C dew point temperature (at 275 kPa). We estimated that at least eight flasks can be sampled (at an overpressure of 275 kPa) with a water vapor content below −2 ∘C dew point temperature during a typical flight sampling up to 5 km altitude over the Amazon, whereas the remaining samples would stay well below 5 ∘C dew point temperature (at 275 kPa). The performance of the air dryer on measurements of CO2, CH4, CO, N2O, and SF6 and the CO2 isotopologues 16O13C16O and 16O12C18O was tested in the laboratory simulating real sampling conditions by compressing humidified air from a calibrated cylinder, after being dried by the air dryer, into sample flasks. We found that the mole fraction and the isotopic composition difference between the different test conditions (including the dryer) and the base condition (dry air, without dryer) remained well within or very close to, in the case of N2O, the World Meteorological Organization recommended compatibility goals for independent measurement programs, proving that the test condition induced no significant bias on the sample measurements.

Transport From the Asian Summer Monsoon Anticyclone Over the Western Pacific

AbstractThe subseasonal scale dynamics of the Asian summer monsoon (ASM) upper troposphere (UT) anticyclone has been identified as a primary mechanism for convectively lofted Asian boundary layer air to leave the confinement of the anticyclone and impact the global UT and lower stratosphere (UTLS). This work quantifies eastward eddy shedding associated with the subseasonal scale oscillation of the anticyclone and associated chemical transport. Using reanalysis data together with satellite trace gas data, we examine the correlation between enhanced tropospheric trace gas species and the presence of a secondary anticyclone over the western Pacific Ocean. To diagnose the role of the western Pacific anticyclone (WPA) in the transport of ASM air into the global UTLS, transport pathways and transit times of air found within the WPA are analyzed using Lagrangian kinematic trajectories. Results show that about two thirds of the air within the WPA originates from, or is influenced by, the greater region of the Tibetan anticyclone. After leaving the WPA, air favors two pathways forward: eastward following the subtropical jet and southwestward following UTLS anticyclonic flow. Approximately 60% of the air parcels cross the tropopause into the lower stratosphere within 30 days, though most cross within a few days. These results highlight opportunities for investigating the impact of the ASM on global UTLS chemical and aerosol composition over the western Pacific via research aircraft.

The Research Unit VolImpact: Revisiting the volcanic impact on atmosphere and climate – preparations for the next big volcanic eruption

This paper provides an overview of the scientific background and the research objectives of the Research Unit “VolImpact” (Revisiting the volcanic impact on atmosphere and climate – preparations for the next big volcanic eruption, FOR 2820). VolImpact was recently funded by the Deutsche Forschungsgemeinschaft (DFG) and started in spring 2019. The main goal of the research unit is to improve our understanding of how the climate system responds to volcanic eruptions. Such an ambitious program is well beyond the capabilities of a single research group, as it requires expertise from complementary disciplines including aerosol microphysical modelling, cloud physics, climate modelling, global observations of trace gas species, clouds and stratospheric aerosols. The research goals will be achieved by building on important recent advances in modelling and measurement capabilities. Examples of the advances in the observations include the now daily near-global observations of multi-spectral aerosol extinction from the limb-scatter instruments OSIRIS, SCIAMACHY and OMPS-LP. In addition, the recently launched SAGE III/ISS and upcoming satellite missions EarthCARE and ALTIUS will provide high resolution observations of aerosols and clouds. Recent improvements in modeling capabilities within the framework of the ICON model family now enable simulations at spatial resolutions fine enough to investigate details of the evolution and dynamics of the volcanic eruptive plume using the large-eddy resolving version, up to volcanic impacts on larger-scale circulation systems in the general circulation model version. When combined with state-of-the-art aerosol and cloud microphysical models, these approaches offer the opportunity to link eruptions directly to their climate forcing. These advances will be exploited in VolImpact to study the effects of volcanic eruptions consistently over the full range of spatial and temporal scales involved, addressing the initial development of explosive eruption plumes (project VolPlume), the variation of stratospheric aerosol particle size and radiative forcing caused by volcanic eruptions (VolARC), the response of clouds (VolCloud), the effects of volcanic eruptions on atmospheric dynamics (VolDyn), as well as their climate impact (VolClim).