Virtue and the Health Professions

Presented to the WMU Center for the Study of Ethics in Society, February 8, 1991

First detection of ammonia (NH₃) in the Asian summer monsoon upper troposphere

Ammonia (NH3) has been detected in the upper troposphere by the analysis of averaged MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) infrared limb-emission spectra. We have found enhanced amounts of NH3 within the region of the Asian summer monsoon at 12–15 km altitude. Three-monthly, 10° longitude  ×  10° latitude average profiles reaching maximum mixing ratios of around 30 pptv in this altitude range have been retrieved, with a vertical resolution of 3–8 km and estimated errors of about 5 pptv. These observations show that loss processes during transport from the boundary layer to the upper troposphere within the Asian monsoon do not deplete the air entirely of NH3. Thus, ammonia might contribute to the so-called Asian tropopause aerosol layer by the formation of ammonium aerosol particles. On a global scale, outside the monsoon area and during different seasons, we could not detect enhanced values of NH3 above the actual detection limit of about 3–5 pptv. This upper bound helps to constrain global model simulations

Retrieval of Water Vapour Profiles from GLORIA Nadir Observations

We present the first analysis of water vapour profiles derived from nadir measurements by the infrared imaging Fourier transform spectrometer GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere). The measurements were performed on 27 September 2017, during the WISE (Wave driven ISentropic Exchange) campaign aboard the HALO aircraft over the North Atlantic in an area between 37°–50°N and 20°–28°W. From each nadir recording of the 2-D imaging spectrometer, the spectral radiances of all non-cloudy pixels have been averaged after application of a newly developed cloud filter. From these mid-infrared nadir spectra, vertical profiles of H2O have been retrieved with a vertical resolution corresponding to five degrees of freedom below the aircraft. Uncertainties in radiometric calibration, temperature and spectroscopy have been identified as dominating error sources. Comparing retrievals resulting from two different a priori assumptions (constant exponential vs. ERA 5 reanalysis data) revealed parts of the flight where the observations clearly show inconsistencies with the ERA 5 water vapour fields. Further, a water vapour inversion at around 6 km altitude could be identified in the nadir retrievals and confirmed by a nearby radiosonde ascent. An intercomparison of multiple water vapour profiles from GLORIA in nadir and limb observational modes, IASI (Infrared Atmospheric Sounding Interferometer) satellite data from two different retrieval processors, and radiosonde measurements shows a broad consistency between the profiles. The comparison shows how fine vertical structures are represented by nadir sounders as well as the influence of a priori information on the retrievals

Differences in ozone retrieval in MIPAS channels A and AB: a spectroscopic issue

Discrepancies in ozone retrievals in MIPAS channels A (685–970cm−1) and AB (1020–1170cm−1) have been a long-standing problem in MIPAS data analysis, amounting to an interchannel bias (AB–A) of up to 8% between ozone volume mixing ratios in the altitude range 30–40km. We discuss various candidate explanations, among them forward model and retrieval algorithm errors, interchannel calibration inconsistencies and spectroscopic data inconsistencies. We show that forward-modelling errors as well as errors in the retrieval algorithm can be ruled out as an explanation because the bias can be reproduced with an entirely independent retrieval algorithm (GEOFIT), relying on a different forward radiative transfer model. Instrumental and calibration issues can also be refuted as an explanation because ozone retrievals based on balloon-borne measurements with a different instrument (MIPAS-B) and an independent level-1 data processing scheme produce a rather similar interchannel bias. Thus, spectroscopic inconsistencies in the MIPAS database used for ozone retrieval are practically the only reason left. To further investigate this issue, we performed retrievals using additional spectroscopic databases. Various versions of the HITRAN database generally produced rather similar channel AB–A differences. Use of a different database, namely GEISA-2015, led to similar results in channel AB, but to even higher ozone volume mixing ratios for channel A retrievals, i.e. to a reversal of the bias. We show that the differences in MIPAS channel A retrievals result from about 13% lower air-broadening coefficients of the strongest lines in the GEISA-2015 database. Since the errors in line intensity of the major lines used in MIPAS channels A and AB are reported to be considerably lower than the observed bias, we posit that a major part of the channel AB–A differences can be attributed to inconsistent air-broadening coefficients as well. To corroborate this assumption we show some clearly inconsistent air-broadening coefficients in the HITRAN-2008 database. The interchannel bias in retrieved ozone amounts can be reduced by increasing the air-broadening coefficients of the lines in MIPAS channel AB in the HITRAN-2008 database by 6%–8%

Biomass burning pollution in the South Atlantic upper troposphere: GLORIA trace gas observations and evaluation of the CAMS model

In this study, we present simultaneous airborne measurements of peroxyacetyl nitrate (PAN), ethane (C2H6), formic acid (HCOOH), methanol (CH3OH), and ethylene (C2H4) above the South Atlantic in September and October 2019. Observations were obtained from the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA), as two-dimensional altitude cross sections along the flight path. The flights were part of the SouthTRAC (Transport and Composition in the Southern Hemisphere Upper Troposphere/Lower Stratosphere) campaign with the German High Altitude and Long Range Research Aircraft (HALO). On two flights (8 September 2019 and 7 October 2019), large enhancements of all these substances were found between 7 and 14 km altitude with maximum volume mixing ratios (VMRs) of 1000 pptv for PAN, 1400 pptv for C2H6, 800 pptv for HCOOH, 4500 pptv for CH3OH, and 200 pptv for C2H4. One flight showed a common filamentary structure in the trace gas distributions, while the second flight is characterized by one large plume. Using backward trajectories, we show that measured pollutants likely reached upper troposphere and lower stratosphere (UTLS) altitudes above South America and central Africa, where elevated PAN VMRs are visible at the surface layer of the Copernicus Atmosphere Monitoring Service (CAMS) model during the weeks before both measurements. In comparison to results of the CAMS reanalysis interpolated onto the GLORIA measurement geolocations, we show that the model is able to reproduce the overall structure of the measured pollution trace gas distributions. For PAN, the absolute VMRs are in agreement with the GLORIA measurements. However, C2H6 and HCOOH are generally underestimated by the model, while CH3OH and C2H4, the species with the shortest atmospheric lifetimes of the pollution trace gases discussed, are overestimated by CAMS. The good agreement between model and observations for PAN suggests that the general transport pathways and emissions locations are well captured by the model. The poorer agreement for other species is therefore most likely linked to model deficiencies in the representation of loss processes and emission strength

Long-term validation of MIPAS ESA operational products using MIPAS-B measurements

The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) was a limb-viewing infrared Fourier transform spectrometer that operated from 2002 to 2012 aboard the Environmental Satellite (ENVISAT). The final re-processing of the full MIPAS mission Level 2 data was performed with the ESA operational version 8 (v8) processor. This MIPAS dataset includes not only the retrieval results of pressure–temperature and the standard species H2O, O3, HNO3, CH4, N2O, and NO2 but also vertical profiles of volume mixing ratios of the more difficult-to-retrieve molecules N2O5, ClONO2, CFC-11, CFC-12 (included since v6 processing), HCFC-22, CCl4, CF4, COF2, and HCN (included since v7 processing). Finally, vertical profiles of the species C2H2, C2H6, COCl2, OCS, CH3Cl, and HDO were additionally retrieved by the v8 processor. The balloon-borne limb-emission sounder MIPAS-B was a precursor of the MIPAS satellite instrument. Several flights with MIPAS-B were carried out during the 10-year operational phase of ENVISAT at different latitudes and seasons, including both operational periods when MIPAS measured with full spectral resolution (FR mode) and with optimised spectral resolution (OR mode). All MIPAS operational products (except HDO) were compared to results inferred from dedicated validation limb sequences of MIPAS-B. To enhance the statistics of vertical profile comparisons, a trajectory match method has been applied to search for MIPAS coincidences along the 2 d forward and backward trajectories running from the MIPAS-B measurement geolocations. This study gives an overview of the validation results based on the ESA operational v8 data comprising the MIPAS FR and OR observation periods. This includes an assessment of the data agreement of both sensors, taking into account the combined errors of the instruments. The differences between the retrieved temperature profiles of both MIPAS instruments generally stays within ±2 K in the stratosphere. For most gases – namely H2O, O3, HNO3, CH4, N2O, NO2, N2O5, ClONO2, CFC-11, CFC-12, HCFC-22, CCl4, CF4, COF2, and HCN – we find a 5 %–20 % level of agreement for the retrieved vertical profiles of both MIPAS instruments in the lower stratosphere. For the species C2H2, C2H6, COCl2, OCS, and CH3Cl, however, larger differences (within 20 %–50 %) appear in this altitude range

The Michelson Interferometer for Passive Atmospheric Sounding global climatology of BrONO2 2002–2012: a test for stratospheric bromine chemistry

We present the first observational dataset of vertically resolved global stratospheric BrONO2 distributions from July 2002 until April 2012 and compare them to results of the atmospheric chemical climate model ECHAM/MESSy Atmospheric Chemistry (EMAC). The retrieved distributions are based on space-borne measurements of infrared limb-emission spectra recorded by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat. The derived vertical profiles of BrONO2 volume mixing ratios represent 10∘ latitude bins and 3 d means, separated into sunlit observations and observations in the dark. The estimated uncertainties are around 1–4 pptv, caused by spectral noise for single profiles as well as for further parameter and systematic errors which may not improve by averaging. Vertical resolutions range from 3 to 8 km between 15 and 35 km altitude. All leading modes of spatial and temporal variability of stratospheric BrONO2 in the observations are well replicated by the model simulations: the large diurnal variability, the low values during polar winter as well as the maximum values at mid and high latitudes during summer. Three major differences between observations and model results are observed: (1) a model underestimation of enhanced BrONO2 in the polar winter stratosphere above about 30 km of up to 15 pptv, (2) up to 8 pptv higher modelled values than observed globally in the lower stratosphere up to 25 km, most obvious during night, and (3) up to 5 pptv lower modelled concentrations at tropical latitudes between 27 and 32 km during sunlit conditions. (1) is explained by the model missing enhanced NOx produced in the mesosphere and lower thermosphere subsiding at high latitudes in winter. This is the first time that observational evidence for enhancement of BrONO2 caused by mesospheric NOx production is reported. The other major inconsistencies (2, 3) between EMAC model results and observations are studied by sensitivity runs with a 1D model. These tentatively hint at a model underestimation of heterogeneous loss of BrONO2 in the lower stratosphere, a simulated production of BrONO2 that is too low during the day as well as strongly underestimated BrONO2 volume mixing ratios when loss via reaction with O(3P) is considered in addition to photolysis. However, considering the uncertainty ranges of model parameters and of measurements, an unambiguous identification of the causes of the differences remains difficult. The observations have also been used to derive the total stratospheric bromine content relative to years of stratospheric entry between 1997 and 2007. With an average value of 21.2±1.4 pptv of Bry at mid latitudes where the modelled adjustment from BrONO2 to Bry is smallest, the MIPAS data agree with estimates of Bry derived from observations of BrO as well as from MIPAS-Balloon measurements of BrONO2.</p