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Stratospheric aerosols are greatly influenced by medium-to-large volcanic eruptions. Over the last few years, extreme wildfires have been identified as new sources of stratospheric particles, in the form of carbonaceous aerosols injected by pyrocumulonimbus (pyroCb) events in the upper troposphere and lower stratosphere, associated with significant impacts on climate and ozone chemistry. To assess the impact of wildfires and volcanic eruptions on stratospheric aerosol loadings in the Northern Hemisphere, the Rapid Balloon Experiments for Sudden Aerosol Injection in the Stratosphere (REAS) project has been initiated. REAS is an international initiative that aims to respond to sudden events impacting stratospheric aerosol composition. Seventeen balloons were launched from Reims, eastern France, between November 2021 and January 2022 to quantify the atmospheric content for both aerosols and trace/greenhouse gases from the ground up to stratospheric levels. The main measurements concerned trace gases (CO/CO2 as tracers of smoke) and aerosol together with ozone using instruments such as a gas collector, optical particle counters, backscatter sondes, an aerosol sampler, an aerosol impactor, and ozonesondes. The Groupe de Spectrométrie Moléculaire et Atmosphérique (GSMA) launch facility provided unique possibilities of combining multiple measurements in one flight thanks to medium flights (corresponding to a 6 kg payload). While no major event impacted the stratosphere during the campaign, we particularly discuss the influence of the aged volcanic plume from La Soufrière volcano (Saint Vincent island) and smoke particles from series of pyroCb events that took place in North America. The burden as well as the optical and microphysical properties of the observed aerosols are quantified from these in situ observations in association with various satellite data. [ABSTRACT FROM AUTHOR]

Observations by CALIPSO have recently been used to identify an aerosol enhancement associated with the Asian Monsoon anticyclone. The Asian Tropopause Aerosol Layer (ATAL) is analogous to observed enhancements in long-lived trace gas species like CO. Since the CALIPSO record only begins in 2006, the question of how long this aerosol feature has been present requires a new look at the long-lived SAGE II data sets despite significant hurdles to its use in the subtropical upper troposphere. We found that a new and more robust method for identifying and eliminating cloud effects from the SAGE II data set was required and, herein, we describe a cloud identification method that appears to capture cloud/aerosol events more effectively than early methods. In addition, we summarize additional challenges to observing the ATAL layer using SAGE II observations. Finally, we perform analyses of the upper troposphere, focusing on periods in which the UTLS is relatively free of volcanic material (1989-1990 and after 1996). We find that there is no evidence of ATAL in the SAGE II data prior to 1998. After 1998, it is clear that aerosol in the upper troposphere in the ATAL region is substantially enhanced relative to the period before that time. In addition, the data generally supports the presence of the ATAL layer beginning in 1999 and continuing through the end of the mission though some years (e.g. 2003) are complicated by the presence of episodic enhancements most likely of volcanic origin. [ABSTRACT FROM AUTHOR]

The trend in stratospheric NO2 column at the NDACC (Network for the Detection of Atmospheric Composition Change) station of Jungfraujoch (46.5° N, 8.0° E) is assessed using ground-based FTIR and zenith-scattered visible sunlight SAOZ measurements over the period 1990 to 2009 as well as a composite satellite nadir data set constructed from ERS-2/GOME, ENVISAT/SCIAMACHY, METOP-A/GOME-2 observations over the 1996-2009 period. To calculate the trends, a linear least squares regression model including explanatory variables for a linear trend, the mean annual cycle, the quasi-biennial oscillation (QBO), solar activity, stratospheric aerosol loading is used. For the 1990-2009 period, statistically indistinguishable trends of -3.7 ± 1.1% decade-1, -3.6 ± decade-11 are derived for the SAOZ and FTIR NO2 column time series, respectively. SAOZ, FTIR, satellite nadir data sets show a similar decrease over the 1996-2009 period, with trends of -2.4 ± 1.1% decade-11, -4.3 ± 1.4% decade-11, and -3.6 ± 2.2% decade-1, respectively. The fact that these declines are opposite in sign to the globally observed +2.5% decade-11 trend in N2O, suggests that factors other than N2O are driving the evolution of stratospheric NO2 at northern mid-latitudes. Possible causes of the decrease in stratospheric NO2 columns have been investigated. The most likely cause is a change in the NO2/NO partitioning in favor of NO, due to a possible stratospheric cooling and a decrease in stratospheric chlorine content, the latter being further confirmed by the negative trend in the ClONO2 column derived from FTIR observations at Jungfraujoch. Decreasing ClO concentrations slows the NO + ClO -> NO2 + Cl reaction and a stratospheric cooling slows the NO + O3 NO2 + O2 reaction, leaving more NOx in the form of NO. The slightly positive trends in ozone estimated from ground- and satellite-based data sets are also consistent with the decrease of NO2 through the NO2 + O3 -> NO3 + O2 reaction. Finally, we cannot rule out the possibility that a strengthening of the Dobson-Brewer circulation, which reduces the time available for N2O photolysis in the stratosphere, could also contribute to the observed decline in stratospheric NO2 above Jungfraujoch. [ABSTRACT FROM AUTHOR]

The trend in stratospheric NO2 column at the NDACC (Network for the Detection of Atmospheric Composition Change) station of Jungfraujoch (46.5° N, 8.0° E) is assessed using ground-based FTIR and zenith-scattered visible sunlight SAOZ measurements over the period 1990 to 2009 as well as a composite satellite nadir data set constructed from ERS-2/GOME, ENVISAT/SCIAMACHY, and METOP-A/GOME-2 observations over the 1996--2009 period. To calculate the trends, a linear least squares regression model including explanatory variables for a linear trend, the mean annual cycle, the quasi-biennial oscillation (QBO), solar activity, and stratospheric aerosol loading is used. For the 1990--2009 period, statistically indistinguishable trends of -3.7±1.1 %/decade and -3.6±0.9 %/decade are derived for the SAOZ and FTIR NO2 column time series, respectively. SAOZ, FTIR, and satellite nadir data sets show a similar decrease over the 1996--2009 period, with trends of -2.4±1.1 %/decade, -4.3±1.4 %/decade, and -3.6±2.2 %/decade, respectively. The fact that these declines are opposite in sign to the globally observed +2.5%/decade trend in N2O, suggests that factors other than N2O are driving the evolution of stratospheric NO2 at northern mid-latitudes. Possible causes of the decrease in stratospheric NO2 columns have been investigated. The most likely cause is a change in the NO2/NO partitioning in favor of NO, due to a possible stratospheric cooling and a decrease in stratospheric chlorine content, the latter being further confirmed by the negative trend in the ClONO2 column derived from FTIR observations at Jungfraujoch. Decreasing ClO concentrations slows the NO+ClO ! NO2 +Cl reaction and a stratospheric cooling slows the NO+O3→NO2 +O2 reaction, leaving more NOx in the form of NO. The slightly positive trends in ozone estimated from ground- and satellite-based data sets are also consistent with the decrease of NO2 through the NO2 +O3→NO3 +O2 reaction. Finally, we cannot rule out the possibility that a strengthening of the Dobson-Brewer circulation, which reduces the time available for N2O photolysis in the stratosphere, could also contribute to the observed decline in stratospheric NO2 above Jungfraujoch. [ABSTRACT FROM AUTHOR]