Abstract. Knowing the spatial and seasonal distributions of nitric acid (HNO3) around the globe is of great interest and allows us to comprehend the processes regulating stratospheric ozone, especially in the polar regions. Due to its unprecedented spatial and temporal sampling, the nadir-viewing Infrared Atmospheric Sounding Interferometer (IASI) is capable of sounding the atmosphere twice a day globally, with good spectral resolution and low noise. With the Fast Optimal Retrievals on Layers for IASI (FORLI) algorithm, we are retrieving, in near real time, columns as well as vertical profiles of several atmospheric species, among which is HNO3. We present in this paper the first characterization of the FORLI-HNO3 profile products, in terms of vertical sensitivity and error budgets. We show that the sensitivity of IASI to HNO3 is highest in the lower stratosphere (10–20 km), where the largest amounts of HNO3 are found, but that the vertical sensitivity of IASI only allows one level of information on the profile (degrees of freedom for signal, DOFS; ∼ 1). The sensitivity near the surface is negligible in most cases, and for this reason, a partial column (5–35 km) is used for the analyses. Both vertical profiles and partial columns are compared to FTIR ground-based measurements from the Network for the Detection of Atmospheric Composition Change (NDACC) to characterize the accuracy and precision of the FORLI-HNO3 product. The profile validation is conducted through the smoothing of the raw FTIR profiles by the IASI averaging kernels and gives good results, with a slight overestimation of IASI measurements in the upper troposphere/lower stratosphere (UTLS) at the six chosen stations (Thule, Kiruna, Jungfraujoch, Izaña, Lauder and Arrival Heights). The validation of the partial columns (5–35 km) is also conclusive with a mean correlation of 0.93 between IASI and the FTIR measurements. An initial survey of the HNO3 spatial and seasonal variabilities obtained from IASI measurements for a 1-year (2011) data set shows that the expected latitudinal gradient of concentrations from low to high latitudes and the large seasonal variability in polar regions (cycle amplitude around 30 % of the seasonal signal, peak to peak) are well represented by IASI data.
Abstract. This study aims to understand the spatial and temporal variability of HNO 3 total columns in terms of explanatory variables. To achieve this, multiple linear regressions are used to fit satellite-derived time series of HNO 3 daily averaged total columns. First, an analysis of the IASI 9-year time series (2008)(2009)(2010)(2011)(2012)(2013)(2014)(2015)(2016) is conducted based on various equivalent latitude bands. The strong and systematic denitrification of the southern polar stratosphere is observed very clearly. It is also possible to distinguish, within the polar vortex, three regions which are differently affected by the denitrification. Three exceptional denitrification episodes in 2011, 2014 and 2016 are also observed in the Northern Hemisphere, due to unusually low arctic temperatures. The time series are then fitted by multivariate regressions to identify what variables are responsible for HNO 3 variability in global distributions and time series, and to quantify their respective influence. Out of an ensemble of proxies (annual cycle, solar flux, quasi-biennial oscillation, multivariate ENSO index, Arctic and Antarctic oscillations and volume of polar stratospheric clouds), only the those defined as significant (p value < 0.05) by a selection algorithm are retained for each equivalent latitude band. Overall, the regression gives a good representation of HNO 3 variability, with especially good results at high latitudes (60-80 % of the observed variability explained by the model). The regressions show the dominance of annual variability in all latitudinal bands, which is related to specific chemistry and dynamics depending on the latitudes. We find that the polar stratospheric clouds (PSCs) also have a major influence in the polar regions, and that their inclusion in the model improves the correlation coefficients and the residuals. However, there is still a relatively large portion of HNO 3 variability that remains unexplained by the model, especially in the intertropical regions, where factors not included in the regression model (such as vegetation fires or lightning) may be at play.
Abstract. Knowing the spatial and seasonal distributions of nitric acid (HNO3) around the globe is of great interest to apprehend the processes regulating stratospheric ozone, especially in the polar regions. Thanks to its unprecedented spatial and temporal sampling, the nadir-viewing Infrared Atmospheric Sounding Interferometer (IASI) allows sounding the atmosphere twice a day globally, with good spectral resolution and low noise. With the Fast Optimal Retrievals on Layers for IASI (FORLI) algorithm, we are retrieving, in near-real time, columns as well as vertical profiles of several atmospheric species, amongst which is HNO3. We present in this paper the first characterization of the FORLI-HNO3 profile products, in terms of vertical sensitivity and error budgets. We show that the sensitivity of IASI to HNO3 is highest in the lower stratosphere (10–20 km), where the largest amounts of HNO3 are found, but that the vertical sensitivity of IASI only allows one level of information on the profile (DOFS 1). The sensitivity near the surface is negligible in most cases, and for this reason, a partial column (5–35 km) is used for the analyses. Both vertical profiles and partial columns are compared to FTIR ground-based measurements from the Network for the Detection of Atmospheric Composition Change (NDACC) to characterize the accuracy and precision of the FORLI-HNO3 product. The profile validation is conducted through the smoothing of the raw FTIR profiles by the IASI averaging kernels and gives good results, with a slight overestimation of IASI measurements in the Upper Troposphere-Lower Stratosphere (UTLS) at the 6 chosen stations (Thule, Kiruna, Jungfraujoch, Izaña, Lauder and Arrival Heights). The validation of the partial columns (5–35 km) is also conclusive with a mean correlation of 0.93 between IASI and the FTIR measurements. An initial survey of the HNO3 spatial and seasonal variabilities obtained from IASI measurements for a one year (2011) data set shows that the expected latitudinal gradient of concentrations from low to high latitudes and the large seasonal variability in polar regions (cycle amplitude around 30 % of the seasonal signal, peak-to-peak) are well represented with IASI data.
Abstract. In this paper, we present the global fingerprint of recent changes in middle–upper stratosphere (MUSt; <25 hPa) ozone (O3) in comparison with lower stratosphere (LSt; 150–25 hPa) O3 derived from the first 10 years of the IASI/Metop-A satellite measurements (January 2008–December 2017). The IASI instrument provides vertically resolved O3 profiles with very high spatial and temporal (twice daily) samplings, allowing O3 changes to be monitored in these two regions of the stratosphere. By applying multivariate regression models with adapted geophysical proxies on daily mean O3 time series, we discriminate anthropogenic trends from various modes of natural variability, such as the El Niño–Southern Oscillation (ENSO). The representativeness of the O3 response to its natural drivers is first examined. One important finding relies on a pronounced contrast between a positive LSt O3 response to ENSO in the extratropics and a negative one in the tropics, with a delay of 3 months, which supports a stratospheric pathway for the ENSO influence on lower stratospheric and tropospheric O3. In terms of trends, we find an unequivocal O3 recovery from the available period of measurements in winter–spring at middle to high latitudes for the two stratospheric layers sounded by IASI (>∼35∘ N–S in the MUSt and >∼45∘ S in the LSt) as well as in the total columns at southern latitudes (>∼45∘ S) where the increase reaches its maximum. These results confirm the effectiveness of the Montreal Protocol and its amendments and represent the first detection of a significant recovery of O3 concurrently in the lower, in the middle–upper stratosphere and in the total column from one single satellite dataset. A significant decline in O3 at northern mid-latitudes in the LSt is also detected, especially in winter–spring of the Northern Hemisphere. Given counteracting trends in the LSt and MUSt at these latitudes, the decline is not categorical in total O3. When freezing the regression coefficients determined for each natural driver over the whole IASI period but adjusting a trend, we calculate a significant speeding up in the O3 response to the decline of O3-depleting substances (ODSs) in the total column, in the LSt and, to a lesser extent, in the MUSt, at high southern latitudes over the year. Results also show a small significant acceleration of the O3 decline at northern mid-latitudes in the LSt and in the total column over the last few years. That, specifically, needs urgent investigation to identify its exact origin and apprehend its impact on climate change. Additional years of IASI measurements would, however, be required to confirm the O3 change rates observed in the stratospheric layers over the last few years.
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