Investigation and amelioration of long-term instrumental drifts in water vapor and nitrous oxide measurements from the Aura Microwave Limb Sounder (MLS) and their implications for studies of variability and trends

The Microwave Limb Sounder (MLS), launched on NASA's Aura spacecraft in 2004, measures vertical profiles of the abundances of key atmospheric species from the upper troposphere to the mesosphere with daily near-global coverage. We review the first 15 years of the record of H2O and N2O measurements from the MLS 190 GHz subsystem (along with other 190 GHz information), with a focus on their long-term stability, largely based on comparisons with measurements from other sensors. These comparisons generally show signs of an increasing drift in the MLS “version 4” (v4) H2O record starting around 2010. Specifically, comparisons with v4.1 measurements from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) indicate a ∼ 2 %–3 % per decade drift over much of the stratosphere, increasing to as much as ∼ 7 % per decade around 46 hPa. Larger drifts, of around 7 %–11 % per decade, are seen in comparisons to balloon-borne frost point hygrometer measurements in the lower stratosphere. Microphysical calculations considering the formation of polar stratospheric clouds in the Antarctic winter stratosphere corroborate a drift in MLS v4 water vapor measurements in that region and season. In contrast, comparisons with the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) instrument on NASA's Thermosphere Ionosphere Mesosphere Energetics and Dynamics (TIMED) mission, and with ground-based Water Vapor Millimeter-wave Spectrometer (WVMS) instruments, do not show statistically significant drifts. However, the uncertainty in these comparisons is large enough to encompass most of the drifts identified in other comparisons. In parallel, the MLS v4 N2O product is shown to be generally decreasing over the same period (when an increase in stratospheric N2O is expected, reflecting a secular growth in emissions), with a more pronounced drift in the lower stratosphere than that found for H2O. Comparisons to ACE-FTS and to MLS N2O observations in a different spectral region, with the latter available from 2004 to 2013, indicate an altitude-dependent drift, growing from 5 % per decade or less in the mid-stratosphere to as much as 15 % per decade in the lower stratosphere. Detailed investigations of the behavior of the MLS 190 GHz subsystem reveal a drift in its “sideband fraction” (the relative sensitivity of the 190 GHz receiver to the two different parts of the microwave spectrum that it observes). Our studies indicate that sideband fraction drift accounts for much of the observed changes in the MLS H2O product and some portion of the changes seen in N2O. The 190 GHz sideband fraction drift has been corrected in the new “version 5” (v5) MLS algorithms, which have now been used to reprocess the entire MLS record. As a result of this correction, the MLS v5 H2O record shows no statistically significant drifts compared to ACE-FTS. However, statistically significant drifts remain between MLS v5 and frost point measurements, although they are reduced. Drifts in v5 N2O are about half the size of those in v4 but remain statistically significant. Scientists are advised to use MLS v5 data in all future studies. Quantification of interregional and seasonal to annual changes in MLS H2O and N2O will not be affected by the drift. However, caution is advised in studies using the MLS record to examine long-term (multiyear) variability and trends in either of these species, especially N2O; such studies should only be undertaken in consultation with the MLS team. Importantly, this drift does not affect any of the MLS observations made in other spectral regions such as O3, HCl, CO, ClO, or temperature.

Investigation and amelioration of long-term instrumental drifts in water vapor and nitrous oxide measurements from the Aura Microwave Limb Sounder (MLS) and their implications for studies of variability and trends

The Microwave Limb Sounder (MLS), launched on NASA's Aura spacecraft in 2004, measures vertical profiles of the abundances of key atmospheric species from the upper troposphere to the mesosphere with daily near-global coverage. We review the first 15 years of the record of H2O and N2O measurements from the MLS 190-GHz subsystem (along with other 190-GHz information), with a focus on their long-term stability, largely based on comparisons with measurements from other sensors. These comparisons generally show signs of an increasing drift in the MLS version 4 (v4) H2O record starting around 2010. Specifically, comparisons with v4.1 measurements from the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS) indicate a ~2–3 %/decade drift over much of the stratosphere, increasing to as much as ~7 %/decade around 46 hPa. Larger drifts, of around 7–11 %/decade, are seen in comparisons to balloon-borne frost point hygrometer measurements in the lower stratosphere. In contrast, the MLS v4 N2O product is shown to be generally decreasing over the same period (when an increase in stratospheric N2O is expected, reflecting a secular growth in emissions), with a more pronounced drift in the lower stratosphere than that found for H2O. Detailed investigations of the behavior of the MLS 190-GHz subsystem reveal a drift in its sideband fraction (the relative sensitivity of the 190-GHz receiver to the two different parts of the microwave spectrum it observes). Our studies indicate that sideband fraction drift accounts for much of the observed changes in the MLS H2O product and some portion of the changes seen in N2O. The 190-GHz sideband fraction drift has been corrected in the new version 5 MLS algorithms, which have now been used to reprocess the entire MLS record. As a result of this correction, the MLS v5 H2O record shows no statistically significant drifts compared to ACE-FTS. However, statistically significant drifts remain between MLS v5 and frost point measurements, though they are reduced. Drifts in v5 N2O are about half the size of those in v4 but remain statistically significant. Scientists are advised to use MLS v5 data in all future studies. Quantification of inter-regional and seasonal-to-annual changes in MLS H2O and N2O will not be affected by the drift. However, caution is advised in studies using the MLS record to examine long-term (multi-year) variability and trends in either of these species, especially N2O; such studies should only be undertaken in consultation with the MLS team. Importantly, this drift does not affect any of the MLS observations made in other spectral regions such as O3, HCl, CO, ClO, or temperature.

Accurate expressions for the dew point and frost point derived from the Rankine-Kirchhoff approximations

Accurate, explicit, and analytic expressions are derived for the dew point and frost point as functions of temperature and relative humidity. These are derived theoretically in terms of physical constants using the Rankine-Kirchhoff approximations, which assume an ideal gas, fixed heat capacities, and zero specific volume of condensates. Compared to modern laboratory measurements, the expressions are accurate to within a few hundredths of a degree over the full range of Earth-relevant temperatures, from 180 to 273 K for the frost point and 230 to 330 K for the dew point.

Understanding balloon-borne frost point hygrometer measurements after contamination by mixed-phase clouds

Balloon-borne water vapour measurements in the upper troposphere and lower stratosphere (UTLS) by means of frost point hygrometers provide important information on air chemistry and climate. However, the risk of contamination from sublimating hydrometeors collected by the intake tube may render these measurements unusable, particularly after crossing low clouds containing supercooled droplets. A large set of (sub)tropical measurements during the 2016–2017 StratoClim balloon campaigns at the southern slopes of the Himalayas allows us to perform an in-depth analysis of this type of contamination. We investigate the efficiency of wall contact and freezing of supercooled droplets in the intake tube and the subsequent sublimation in the UTLS using computational fluid dynamics (CFD). We find that the airflow can enter the intake tube with impact angles up to 60∘, owing to the pendulum motion of the payload. Supercooled droplets with radii > 70 µm, as they frequently occur in mid-tropospheric clouds, typically undergo contact freezing when entering the intake tube, whereas only about 50 % of droplets with 10 µm radius freeze, and droplets < 5 µm radius mostly avoid contact. According to CFD, sublimation of water from an icy intake can account for the occasionally observed unrealistically high water vapour mixing ratios (χH2O > 100 ppmv) in the stratosphere. Furthermore, we use CFD to differentiate between stratospheric water vapour contamination by an icy intake tube and contamination caused by outgassing from the balloon and payload, revealing that the latter starts playing a role only during ascent at high altitudes (p < 20 hPa).

Understanding cryogenic frost point hygrometer measurements after contamination by mixed-phase clouds

Balloon-borne water vapour measurements in the (sub)tropical upper troposphere and lower stratosphere (UTLS) by means of frost point hygrometers provide important information on air chemistry and climate. However, the risk of contamination from sublimating hydrometeors collected by the intake tube may render these measurements difficult, particularly after crossing low clouds containing supercooled droplets. A large set of measurements during the 2016–2017 StratoClim balloon campaigns at the southern slopes of the Himalayas allows us to perform an in-depth analysis of this type of contamination. We investigate the efficiency of wall-contact and freezing of supercooled droplets in the intake tube and the subsequent sublimation in the UTLS using Computational Fluid Dynamics (CFD). We find that the airflow can enter the intake tube with impingement angles up to 60°, owing to the pendulum motion of the payload. Supercooled droplets with radii > 70 μm, as they frequently occur in mid-tropospheric clouds, typically undergo contact freezing when entering the intake tube, whereas only about 50 % of droplets with 10 μm radius freeze, and droplets 100 ppmv) in the stratosphere. Furthermore, we use CFD to differentiate between stratospheric water vapour contamination by an icy intake tube and contamination caused by outgassing from the balloon and payload, revealing that the latter starts playing a role only at high altitudes (p