scholarly journals Photolysis controls the isotopic composition of water products escaping Mars’ atmosphere

2021 ◽  
Author(s):  
Juan Alday ◽  
Alexander Trokhimovskiy ◽  
Patrick Irwin ◽  
Colin Wilson ◽  
Franck Montmessin ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Isotope Composition ◽  
Relative Proportion ◽  
Upper Atmosphere ◽  
Trace Gas ◽  
Main Process ◽  
Deuterated Water ◽  
Ion Chemistry ◽  
Mars Atmosphere ◽  
Photolysis Rates

Abstract The current Martian atmosphere is about five times more enriched in deuterium than Earth's, providing a direct testimony that Mars hosted several times more water in its early youth than nowadays. Estimates of the total amount of water lost to space from the current mean D/H value depend on a rigorous appraisal of the relative escape between deuterated and non-deuterated water. The transport of water to the upper atmosphere, from whence it may escape to space, has been assumed to be controlled by water condensation and photolysis, both of which affect the isotope composition of the escaping hydrogen. Their respective role in influencing the relative proportion of escaping D and H atom populations in the upper atmosphere has remained speculative. Here we report HDO and H<2sub>O profiles observed by the Atmospheric Chemistry Suite (ExoMars Trace Gas Orbiter) in orbit around Mars that, once combined with expected photolysis rates, reveal that the ultraviolet dissociation of water not only governs the production of atomic hydrogen, prevailing over the ion chemistry mechanism, but also dominates the production of H relative to D atoms, disrupting the old paradigm of atmospheric condensation being the main process differentiating D and H in the upper atmosphere.

Composition and chemistry of Titan's thermosphere and ionosphere

2008 ◽  
Vol 367 (1889) ◽  
pp. 729-741 ◽  
Author(s):  
V Vuitton ◽  
R.V Yelle ◽  
P Lavvas
Keyword(s):  
Atmospheric Chemistry ◽  
Recent Progress ◽  
Organic Aerosols ◽  
Direct Consequence ◽  
Upper Atmosphere ◽  
Ion Chemistry ◽  
Lower Altitude ◽  
Positive Ions ◽  
Aromatic Species ◽  
Plasma Spectrometer

Titan has long been known to harbour the richest atmospheric chemistry in the Solar System. Until recently, it had been believed that complex hydrocarbons and nitriles were produced through neutral chemistry that would eventually lead to the formation of micrometre sized organic aerosols. However, recent measurements by the Cassini spacecraft are drastically changing our understanding of Titan's chemistry. The Ion and Neutral Mass Spectrometer (INMS) and the Cassini Plasma Spectrometer (CAPS) revealed an extraordinary complex ionospheric composition. INMS detected roughly 50 positive ions with m / z <100 and a density higher than 0.1 cm −3 . CAPS provided evidence for heavy (up to 350 amu) positively and negatively charged (up to 4000 amu) ions. These observations all indicate that Titan's ionospheric chemistry is incredibly complex and that molecular growth starts in the upper atmosphere rather than at lower altitude. Here, we review the recent progress made on ionospheric chemistry. The presence of heavy neutrals in the upper atmosphere has been inferred as a direct consequence of the presence of complex positive ions. Benzene (C 6 H 6 ) is created by ion chemistry at high altitudes and its main photolysis product, the phenyl radical (C 6 H 5 ), is at the origin of the formation of aromatic species at lower altitude.

scholarly journals Stormy water on Mars: The distribution and saturation of atmospheric water during the dusty season

Science ◽  
2020 ◽  
Vol 367 (6475) ◽  
pp. 297-300 ◽  
Author(s):  
Anna A. Fedorova ◽  
Franck Montmessin ◽  
Oleg Korablev ◽  
Mikhail Luginin ◽  
Alexander Trokhimovskiy ◽  
...  
Keyword(s):  
High Altitude ◽  
Atmospheric Chemistry ◽  
Water Distribution ◽  
Upper Atmosphere ◽  
Trace Gas ◽  
Atmospheric Water ◽  
Water On Mars

The loss of water from Mars to space is thought to result from the transport of water to the upper atmosphere, where it is dissociated to hydrogen and escapes the planet. Recent observations have suggested large, rapid seasonal intrusions of water into the upper atmosphere, boosting the hydrogen abundance. We use the Atmospheric Chemistry Suite on the ExoMars Trace Gas Orbiter to characterize the water distribution by altitude. Water profiles during the 2018–2019 southern spring and summer stormy seasons show that high-altitude water is preferentially supplied close to perihelion, and supersaturation occurs even when clouds are present. This implies that the potential for water to escape from Mars is higher than previously thought.

scholarly journals Impact of uncertainties in inorganic chemical rate constants on tropospheric composition and ozone radiative forcing

2017 ◽  
Author(s):  
Ben Newsome ◽  
Mat Evans
Keyword(s):  
Rate Constant ◽  
Atmospheric Chemistry ◽  
Rate Constants ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Surface Ozone ◽  
Photolysis Rates ◽  
The Impact ◽  
Chemical Rate

Abstract. Chemical rate constants determine the composition of the atmosphere and how this composition has changed over time. They are central to our understanding of climate change and air quality degradation. Atmospheric chemistry models, whether online or offline, box, regional or global use these rate constants. Expert panels synthesise laboratory measurements, making recommendations for the rate constants that should be used. This results in very similar or identical rate constants being used by all models. The inherent uncertainties in these recommendations are, in general, therefore ignored. We explore the impact of these uncertainties on the composition of the troposphere using the GEOS-Chem chemistry transport model. Based on the JPL and IUPAC evaluations we assess 50 mainly inorganic rate constants and 10 photolysis rates, through simulations where we increase the rate of the reactions to the 1σ upper value recommended by the expert panels. We assess the impact on 4 standard metrics: annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime. Uncertainty in the rate constants for NO2 + OH    M →  HNO3, OH + CH4 → CH3O2 + H2O and O3 + NO → NO2 + O2 are the three largest source of uncertainty in these metrics. We investigate two methods of assessing these uncertainties, addition in quadrature and a Monte Carlo approach, and conclude they give similar outcomes. Combining the uncertainties across the 60 reactions, gives overall uncertainties on the annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime of 11, 12, 17 and 17 % respectively. These are larger than the spread between models in recent model inter-comparisons. Remote regions such as the tropics, poles, and upper troposphere are most uncertain. This chemical uncertainty is sufficiently large to suggest that rate constant uncertainty should be considered when model results disagree with measurement. Calculations for the pre-industrial allow a tropospheric ozone radiative forcing to be calculated of 0.412 ± 0.062 Wm−2. This uncertainty (15 %) is comparable to the inter-model spread in ozone radiative forcing found in previous model-model inter-comparison studies where the rate constants used in the models are all identical or very similar. Thus the uncertainty of tropospheric ozone radiative forcing should expanded to include this additional source of uncertainty. These rate constant uncertainties are significant and suggest that refinement of supposedly well known chemical rate constants should be considered alongside other improvements to enhance our understanding of atmospheric processes.

scholarly journals Case studies of the impact of orbital sampling on stratospheric trend detection and derivation of tropical vertical velocities: solar occultation vs. limb emission sounding

2016 ◽  
Vol 16 (18) ◽  
pp. 11521-11534 ◽  
Author(s):  
Luis F. Millán ◽  
Nathaniel J. Livesey ◽  
Michelle L. Santee ◽  
Jessica L. Neu ◽  
Gloria L. Manney ◽  
...  
Keyword(s):  
Case Studies ◽  
Atmospheric Chemistry ◽  
Stratospheric Ozone ◽  
Sampling Bias ◽  
Nonuniform Sampling ◽  
Trend Detection ◽  
Trace Gas ◽  
Uniform Sampling ◽  
Solar Occultation ◽  
The Impact

Abstract. This study investigates the representativeness of two types of orbital sampling applied to stratospheric temperature and trace gas fields. Model fields are sampled using real sampling patterns from the Aura Microwave Limb Sounder (MLS), the HALogen Occultation Experiment (HALOE) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). The MLS sampling acts as a proxy for a dense uniform sampling pattern typical of limb emission sounders, while HALOE and ACE-FTS represent coarse nonuniform sampling patterns characteristic of solar occultation instruments. First, this study revisits the impact of sampling patterns in terms of the sampling bias, as previous studies have done. Then, it quantifies the impact of different sampling patterns on the estimation of trends and their associated detectability. In general, we find that coarse nonuniform sampling patterns may introduce non-negligible errors in the inferred magnitude of temperature and trace gas trends and necessitate considerably longer records for their definitive detection. Lastly, we explore the impact of these sampling patterns on tropical vertical velocities derived from stratospheric water vapor measurements. We find that coarse nonuniform sampling may lead to a biased depiction of the tropical vertical velocities and, hence, to a biased estimation of the impact of the mechanisms that modulate these velocities. These case studies suggest that dense uniform sampling such as that available from limb emission sounders provides much greater fidelity in detecting signals of stratospheric change (for example, fingerprints of greenhouse gas warming and stratospheric ozone recovery) than coarse nonuniform sampling such as that of solar occultation instruments.

scholarly journals Dynamics and composition of the Asian summer monsoon anticyclone

2017 ◽  
Author(s):  
Klaus-Dirk Gottschaldt ◽  
Hans Schlager ◽  
Robert Baumann ◽  
Duy S. Cai ◽  
Veronika Eyring ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
Atmospheric Chemistry ◽  
Asian Summer Monsoon ◽  
Monsoon Season ◽  
Lower Troposphere ◽  
Equatorial Region ◽  
Ozone Production ◽  
Trace Gas ◽  
Asian Summer ◽  
Southern Fringe

Abstract. This study places HALO research aircraft observations in the upper-tropospheric Asian summer monsoon anticyclone (ASMA) obtained during the Earth System Model Validation (ESMVal) campaign in September 2012 into the context of regional, intra-annual variability by hindcasts with the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. The simulations demonstrate that tropospheric trace gas profiles in the monsoon season are distinct from the rest of the year. Air uplifted from the lower troposphere to the tropopause layer dominates the eastern part of the ASMA’s interior, while the western part is characterised by subsidence down to the mid-troposphere. Soluble compounds are being washed out when uplifted by convection in the eastern part, where lightning simultaneously replenishes reactive nitrogen in the upper troposphere. Net photochemical ozone production is significantly enhanced in the ASMA, contrasted by an ozone depleting regime in the mid-troposphere and more neutral conditions in autumn and winter. An analysis of multiple monsoon seasons in the simulation shows that stratospherically influenced tropopause layer air is regularly entrained at the eastern ASMA flank, and then transported in the southern fringe around the interior region. Observed and simulated tracer-tracer relations reflect photochemical O3 production, as well as in-mixing from the lower troposphere and the tropopause layer. The simulation additionally shows entrainment of clean air from the equatorial region by northerly winds at the western ASMA flank. Although the in situ measurements were performed towards the end of summer, the main ingredients needed for their interpretation are present throughout the monsoon season. A transition between two dynamical modes of the ASMA took place during the HALO ESMVal campaign. Transport barriers of the original anticyclone are overcome effectively when it splits up. Air from the fringe is stirred into the interiors of the new anticyclones and vice versa. Instabilities of this and other types occur quite frequently. Our study emphasises their paramountcy for the trace gas composition of the ASMA and its outflow into regions around the world.

scholarly journals The high Arctic in extreme winters: vortex, temperature, and MLS and ACE-FTS trace gas evolution

2008 ◽  
Vol 8 (3) ◽  
pp. 505-522 ◽  
Author(s):  
G. L. Manney ◽  
W. H. Daffer ◽  
K. B. Strawbridge ◽  
K. A. Walker ◽  
C. D. Boone ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
High Arctic ◽  
Trace Gas ◽  
Satellite Measurements ◽  
Broadband Emission ◽  
Gas Measurements ◽  
Chemistry Experiment ◽  
Very High ◽  
Good Agreement

Abstract. The first three Arctic winters of the ACE mission represented two extremes of winter variability: Stratospheric sudden warmings (SSWs) in 2004 and 2006 were among the strongest, most prolonged on record; 2005 was a record cold winter. Canadian Arctic Atmospheric Chemistry Experiment (ACE) Validation Campaigns were conducted at Eureka (80° N, 86° W) during each of these winters. New satellite measurements from ACE-Fourier Transform Spectrometer (ACE-FTS), Sounding of the Atmosphere using Broadband Emission Radiometry (SABER), and Aura Microwave Limb Sounder (MLS), along with meteorological analyses and Eureka lidar temperatures, are used to detail the meteorology in these winters, to demonstrate its influence on transport, and to provide a context for interpretation of ACE-FTS and validation campaign observations. During the 2004 and 2006 SSWs, the vortex broke down throughout the stratosphere, reformed quickly in the upper stratosphere, and remained weak in the middle and lower stratosphere. The stratopause reformed at very high altitude, near 75 km. ACE measurements covered both vortex and extra-vortex conditions in each winter, except in late-February through mid-March 2004 and 2006, when the strong, pole-centered vortex that reformed after the SSWs resulted in ACE sampling only inside the vortex in the middle through upper stratosphere. The 2004 and 2006 Eureka campaigns were during the recovery from the SSWs, with the redeveloping vortex over Eureka. 2005 was the coldest winter on record in the lower stratosphere, but with an early final warming in mid-March. The vortex was over Eureka at the start of the 2005 campaign, but moved away as it broke up. Disparate temperature profile structure and vortex evolution resulted in much lower (higher) temperatures in the upper (lower) stratosphere in 2004 and 2006 than in 2005. Satellite temperatures agree well with lidar data up to 50–60 km, and ACE-FTS, MLS and SABER show good agreement in high-latitude temperatures throughout the winters. Consistent with a strong, cold upper stratospheric vortex and enhanced radiative cooling after the SSWs, MLS and ACE-FTS trace gas measurements show strongly enhanced descent in the upper stratospheric vortex in late January through March 2006 compared to that in 2005.

scholarly journals Validation of MIPAS IMK/IAA methane profiles

2015 ◽  
Vol 8 (12) ◽  
pp. 5251-5261 ◽  
Author(s):  
A. Laeng ◽  
J. Plieninger ◽  
T. von Clarmann ◽  
U. Grabowski ◽  
G. Stiller ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Michelson Interferometer ◽  
European Space Agency ◽  
Trace Gas ◽  
Mixing Ratios ◽  
Air Sampler ◽  
Solar Occultation ◽  
Space Agency ◽  
Scanning Imaging ◽  
Satellite Instruments

Abstract. The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) is an infrared (IR) limb emission spectrometer on the Envisat platform. It measures trace gas distributions during day and night, pole-to-pole, over an altitude range from 6 to 70 km in nominal mode and up to 170 km in special modes, depending on the measurement mode, producing more than 1000 profiles day−1. We present the results of a validation study of methane, version V5R_CH4_222, retrieved with the IMK/IAA (Institut für Meteorologie und Klimaforschung, Karlsruhe/Instituto de Astrofisica de Andalucia, Grenada) MIPAS scientific level 2 processor. The level 1 spectra are provided by the ESA (European Space Agency) and version 5 was used. The time period covered is 2005–2012, which corresponds to the period when MIPAS measured trace gas distributions at a reduced spectral resolution of 0.0625 cm−1. The comparison with satellite instruments includes the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), the HALogen Occultation Experiment (HALOE), the Solar Occultation For Ice Experiment (SOFIE) and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY). Furthermore, comparisons with MkIV balloon-borne solar occultation measurements and with air sampling measurements performed by the University of Frankfurt are presented. The validation activities include bias determination, assessment of stability, precision validation, analysis of histograms and comparison of corresponding climatologies. Above 50 km altitude, MIPAS methane mixing ratios agree within 3 % with ACE-FTS and SOFIE. Between 30 and 40 km an agreement within 3 % with SCIAMACHY has been found. In the middle stratosphere, there is no clear indication of a MIPAS bias since comparisons with various instruments contradict each other. In the lower stratosphere (below 25 km) MIPAS CH4 is biased high with respect to satellite instruments, and the most likely estimate of this bias is 14 %. However, in the comparison with CH4 data obtained from cryogenic whole-air sampler (cryosampler) measurements, there is no evidence of a high bias in MIPAS between 20 and 25 km altitude. Precision validation is performed on collocated MIPAS–MIPAS pairs and suggests a slight underestimation of its uncertainties by a factor of 1.2. No significant evidence of an instrumental drift has been found.

scholarly journals First detection of ozone in the mid-infrared at Mars: implications for methane detection

2020 ◽  
Vol 639 ◽  
pp. A141 ◽  
Author(s):  
K. S. Olsen ◽  
F. Lefèvre ◽  
F. Montmessin ◽  
A. Trokhimovskiy ◽  
L. Baggio ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Polar Vortex ◽  
Trace Gas ◽  
Spectral Signature ◽  
Infrared Range ◽  
Mid Infrared ◽  
Northern Latitudes ◽  
Ultraviolet Range ◽  
Vibration Rotation ◽  
Methane Detection

Aims. The ExoMars Trace Gas Orbiter was sent to Mars in March 2016 to search for trace gases diagnostic of active geological or biogenic processes. Methods. We report the first observation of the spectral features of Martian ozone (O3) in the mid-infrared range using the Atmospheric Chemistry Suite Mid-InfaRed (MIR) channel, a cross-dispersion spectrometer operating in solar occultation mode with the finest spectral resolution of any remote sensing mission to Mars. Results. Observations of ozone were made at high northern latitudes (>65°N) prior to the onset of the 2018 global dust storm (Ls = 163–193°). During this fast transition phase between summer and winter ozone distribution, the O3 volume mixing ratio observed is 100–200 ppbv near 20 km. These amounts are consistent with past observations made at the edge of the southern polar vortex in the ultraviolet range. The observed spectral signature of ozone at 3000–3060 cm−1 directly overlaps with the spectral range of the methane (CH4) ν3 vibration-rotation band, and it, along with a newly discovered CO2 band in the same region, may interfere with measurements of methane abundance.

scholarly journals Estimate of the D/H ratio in the Martian upper atmosphere from the low spectral resolution mode of MAVEN/IUVS

2020 ◽  
Author(s):  
Jean-Yves Chaufray ◽  
Majd Mayyasi ◽  
Michael Chaffin ◽  
Justin Deighan ◽  
Dolon Bhattacharyya ◽  
...  
Keyword(s):  
High Resolution ◽  
Spectral Resolution ◽  
Quantitative Information ◽  
Upper Atmosphere ◽  
Vertical Profiles ◽  
Low Resolution ◽  
Mars Atmosphere

&lt;p&gt;The recent observations performed with the high-resolution &amp;#8220;echelle mode&amp;#8221; by the Imaging Ultraviolet Spectrograph (IUVS) aboard the Mars Atmosphere and Volatile EvolutioN (MAVEN) mission indicated large deuterium brightness near Ls=270&amp;#176;. The deuterium brightness observed at the beginning of the mission, when Mars was close to its perihelion show brightness ~ 1 kR much larger than the first deuterium detection from Earth ~ 20-50R in 20-21 January 1997 (Ls = 67&amp;#176;). This low brightness of the deuterium emission is consistent with the lack of deuterium observation with the echelle mode of IUVS at solar longitudes around aphelion (Ls = 71&amp;#176;). During southern summer (Ls = 270&amp;#176;), especially near the terminator, the Lyman-&amp;#945; emission observed at 121.6 nm with the &amp;#8220;low resolution mode&amp;#8221; presents some vertical profiles that were not reproducible with models including only the emission from the thermal hydrogen population. In this study, we investigate the possibility to derive quantitative information on the D/H ratio at Mars from the vertical Lyman-&amp;#945; profiles observed with the &amp;#8220;low resolution mode&amp;#8221;, and the main limits of the method.&lt;/p&gt;

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