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Odd-hydrogen (HO |$_\mathrm{x}$|⁠) species have a crucial role in regulating the chemistry of the atmosphere of Mars and are important to understand some of the most fundamental aspects regarding its atmospheric composition such as the long-term stability of CO |$_2$|⁠. Despite the key role of these species for our understanding of the Martian photochemistry, there is little observational evidence constraining their abundances. In this study, we use infrared solar occultation observations from the Atmospheric Chemistry Suite aboard the ExoMars Trace Gas Orbiter to search for spectral signatures of HO |$_2$| in the atmosphere of Mars. In our analysis of the data, we retrieve vertical profiles of pressure, temperature, and water vapour mixing ratio, but are unable to confidently detect the presence of HO |$_2$| features in the spectra. We report upper limits of 15 ppbv (5 |$\sigma$|⁠), which represents an order of magnitude improvement with respect to previous investigations. Comparing the derived upper limits with the expectations from 3-dimensional Global Climate Models, we find that approximately an order of magnitude improvement in the instrument sensitivity would be required to detect this molecule and/or constrain the models. [ABSTRACT FROM AUTHOR]

On Mars, condensation is the major factor constraining the vertical distribution of water vapor. Recent measurements of water and temperature profiles showed that water can be strongly supersaturated at and above the level where clouds form during the aphelion and perihelion seasons. Since 2018, the near‐infrared spectrometer (NIR) of the Atmospheric Chemistry Suite onboard the Trace Gas Orbiter has measured H2O and temperature profiles using solar occultation in the infrared from below 10 to 100 km of altitude. Here, we provide the first long‐term monitoring of the water saturation state. The survey spans 2 Martian years from Ls = 163° of MY34 to Ls = 170° of MY36. We found that water is often supersaturated above aerosol layers. In the aphelion season, the water mixing ratio above 40 km in the mid‐to‐high latitudes was below 3 ppmv and yet is found to be supersaturated. Around the perihelion, water is also supersaturated above 60 km with a mixing ratio of 30–50 ppmv. Stronger saturation is observed during the dusty season in MY35 compared to what was observed in MY34 during the Global Dust Storm and around the perihelion. Saturation varied between the evening and morning terminators in response to temperature modulation imparted by thermal tides. Although water vapor is more abundant in the evening, colder morning temperatures induce a daily peak of saturation. This data set establishes a new paradigm for water vapor on Mars, revealing that supersaturation is nearly ubiquitous, particularly during the dust season, thereby promoting water escape on an annual average. Plain Language Summary: The rate of water loss from Mars depends on hydrogen, the main product of the H2O photodissociation escaping from the upper atmosphere. The ability of water to reach high altitudes and to be a direct source of atomic hydrogen is limited by cloud formation, which holds water vapor in the lower atmosphere. This process is regulated by temperature and pressure. Condensation starts when the temperature is cold enough and condensation nuclei (CN) (e.g., small dust particles) are available. If CN are lacking, or their sizes are too small, or the temperature drops too fast, then water vapor becomes supersaturated. Recent studies have shown that Martian water vapor is often supersaturated. Here, we present the first seasonal cycle of the saturation state from simultaneous measurements of water and temperature during two Martian years by Atmospheric Chemistry Suite on the Trace Gas Orbiter. Our results show that supersaturation is typical on Mars. It occurs above clouds both in the aphelion and perihelion seasons as well as in the lower polar atmosphere. We demonstrate supersaturation to be an important factor facilitating the escape of water. Unlike the Earth, water easily penetrates the upper atmosphere and reaches photodissociation altitudes. Key Points: Long‐term observations of H2O saturation state in the atmosphere of Mars show that supersaturation is nearly ubiquitous above aerosol layersDuring the dusty season, the supersaturation is stronger in MY35 compared to MY34More water was found in the evening terminator and stronger supersaturation in the morning terminator [ABSTRACT FROM AUTHOR]

Isotopic ratios in atmospheric CO2 are shaped by various processes throughout Mars' history, and can help understand what the atmosphere of early Mars was like to sustain liquid water on its surface. In this study, we monitor the O and C isotopic composition of CO2 between 70 and 130 km for more than half a Martian year using solar occultation observations by the Atmospheric Chemistry Suite onboard the ExoMars Trace Gas Orbiter. We find the vertical trends of the isotopic ratios to be consistent with the expectations from diffusive separation above the homopause, with average values below this altitude being consistent with Earth‐like fractionation (δ13C = −3 ± 37‰; δ18O = −29 ± 38‰; and δ17O = −11 ± 41‰). Using these measurements, we estimate that at least 20%–40% of primordial C on Mars has escaped to space throughout history. The total amount of C lost from the atmosphere is likely to be well in excess of this lower limit, due to carbonate formation and further sink processes. In addition, we propose a photochemical transfer of light O from H2O to CO2 to explain the larger enrichment in the O18/O16 ${}^{18}\mathrm{O}/{}^{16}\mathrm{O}$ ratio in H2O than in CO2. Plain Language Summary: There is ample evidence suggesting that liquid water was abundant on the surface of Mars in the past. However, climatic conditions on early Mars must have been very different from the ones we observe today to sustain liquid water on its surface. The ratios of the heavy and light isotopes in different species provide a very useful tool to estimate the early climate of Mars. In this study, we monitor the isotopic ratios of carbon dioxide in the atmosphere of Mars to provide more accurate estimates of these. With our measurements, and in context with previous studies, we estimate that at least 20%–40% of the carbon reservoir has been lost to space throughout Martian history. This, together with the sequestration of atmospheric C on the surface in the form of minerals, is consistent with the idea that the atmosphere of early Mars was denser than the one we observe today. Key Points: Isotopic ratios in CO2 are observed to be consistent with telluric standards and to fractionate by diffusive separation above the homopauseAt least 20%–40% of the C reservoir has escaped to space throughout Martian historyThe higher 18O/16O ratio in H2O than in CO2 may be explained by a photochemical transfer of lighter O from H2O to CO2 [ABSTRACT FROM AUTHOR]