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The reaction of CH ₄ with chlorine (Cl) radicals in the atmosphere is associated with an extraordinarily strong isotopic fractionation, where ¹2 CH ₄ reacts about 70 ‰ faster with Cl than ¹3 CH ₄ . Therefore, although the Cl-based sink of CH ₄ constitutes only a small contribution to its total removal rate, the uncertainty in this small sink has been identified as one of the two largest uncertainties of isotope-based CH ₄ source apportionment at the global scale. The uncertainty arises from the fact that Cl levels in the atmosphere are so low that they cannot be detected directly. One very sensitive indirect method to identify and quantify the CH ₄ + Cl reaction in the atmosphere is the detection of the extremely ¹3 C-depleted reaction product carbon monoxide (CO) from this reaction. This article reviews the concept of this approach, its successful application in the atmosphere, its challenges and opportunities for identifying and quantifying Cl-based removal of CH ₄ at the regional and global scale and its potential to detect and evaluate possible attempts to enhance CH ₄ removal from the atmosphere.

The volcanic eruption of Cumbre Vieja (La Palma Island, Spain), started on 19 September, 2021, and was declared terminated on 25 December, 2021. A complete set of aerosol measurements were deployed around the volcano within the first month of the eruptive activity. This paper describes the results of the observations made at Tazacorte on the west bank of the island where a polarized micro pulse lidar was deployed. The two and a half months analyzed (16 October – 31 December) reveal that the peak height of the lowermost and strongest volcanic plume did not exceed 3 km (mean of 1.43±0.45 km over the whole period) and was highly variable. It steadily increased until week 11 after the eruption start (and 3 weeks before its end) and started decreasing afterwards. The ash mass concentration has been assessed with a method based on the polarization capability of the instrument. Considering the limitation of current remote sensing techniques to detect large to giant particles, the ash mass concentration on one of the days with the highest ash load is estimated to have peaked in the range 800-3200 μg m(exp -3) in the lowermost layer below 2.5 km.

Following the emergence of the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) responsible for COVID-19 in December 2019 in Wuhan (China) and its spread to the rest of the world, the World Health Organization declared a global pandemic in March 2020. Without effective treatment in the initial pandemic phase, social distancing and mandatory quarantines were introduced as the only available preventative measure. In contrast to the detrimental societal impacts, air quality improved in all countries in which strict lockdowns were applied, due to lower pollutant emissions. Here we investigate the effects of the COVID-19 lockdowns in Europe on ambient black carbon (BC), which affects climate and damages health, using in situ observations from 17 European stations in a Bayesian inversion framework. BC emissions declined by 23 kt in Europe (20 % in Italy, 40 % in Germany, 34 % in Spain, 22 % in France) during lockdowns compared to the same period in the previous 5 years, which is partially attributed to COVID-19 measures. BC temporal variation in the countries enduring the most drastic restrictions showed the most distinct lockdown impacts. Increased particle light absorption in the beginning of the lockdown, confirmed by assimilated satellite and remote sensing data, suggests residential combustion was the dominant BC source. Accordingly, in central and Eastern Europe, which experienced lower than average temperatures, BC was elevated compared to the previous 5 years. Nevertheless, an average decrease of 11 % was seen for the whole of Europe compared to the start of the lockdown period, with the highest peaks in France (42 %), Germany (21 %), UK (13 %), Spain (11 %) and Italy (8 %). Such a decrease was not seen in the previous years, which also confirms the impact of COVID-19 on the European emissions of BC.

In order to assess the evolution of aerosol parameters affecting climate change, a long-term trend analysis of aerosol optical properties was performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann–Kendall (MK) statistical test associated with several pre-whitening methods and with Sen's slope was used as the main trend analysis method. Comparisons with general least mean square associated with autoregressive bootstrap (GLS/ARB) and with standard least mean square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficient trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficient time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, eastern/northern Europe and the Arctic, 22 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 26 % of sites have trends which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10-year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10-year trends are primarily found for earlier periods (10-year trends ending in 2010–2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10-year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10-year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10-year trends of the scattering coefficient – there is a shift to statistically significant negative trends in 2009–2012 for all stations in the eastern and central USA. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage provides insight into potential aerosol effects on climate changes.

Tropospheric ozone trends from models and satellites are found to diverge. Ground-based (GB) observations are used to reference models and satellites, but GB data themselves might display station biases and discontinuities. Reprocessing with uniform procedures, the TOAR-II working group Harmonization and Evaluation of Ground-based Instruments for Free-Tropospheric Ozone Measurements (HEGIFTOM) homogenized public data from five networks: ozonesondes, In-service Aircraft for a Global Observing System (IAGOS) profiles, solar absorption Fourier transform infrared (FTIR) spectrometer measurements, lidar observations, and Dobson Umkehr data. Amounts and uncertainties for total tropospheric ozone (TrOC; surface to 300 hPa), as well as free- and lower-tropospheric ozone, are calculated for each network. We report trends (2000 to 2022) for these segments using quantile regression (QR) and multiple linear regression (MLR) for 55 datasets, including six multi-instrument stations. The findings are that (1) median TrOC trends computed with QR and MLR trends are essentially the same; (2) pole-to-pole, across all longitudes, TrOC trends fall within +3 to −3 ppbv per decade, equivalent to (−4 % to +8 %) per decade depending on site; (3) the greatest fractional increases occur over most tropical and subtropical sites, with decreases at northern high latitudes, but these patterns are not uniform; (4) post-COVID trends are smaller than pre-COVID trends for Northern Hemisphere mid-latitude sites. In summary, this analysis conducted in the frame of TOAR-II/HEGIFTOM shows that high-quality, multi-instrument, harmonized data over a wide range of ground sites provide clear standard references for TOAR-II models and evolving tropospheric ozone satellite products for 2000–2022.

High-resolution Fourier transform infrared (FTIR) solar observations are particularly relevant for climate studies, as they allow atmospheric gaseous composition and multiple climate processes to be monitored in detail. In this context, the present paper provides an overview of 20 years of FTIR measurements taken in the framework of the NDACC (Network for the Detection of Atmospheric Composition Change) from 1999 to 2018 at the subtropical Izaña Observatory (IZO, Spain). Firstly, long-term instrumental performance is comprehensively assessed, corroborating the temporal stability and reliable instrumental characterization of the two FTIR spectrometers installed at IZO since 1999. Then, the time series of all trace gases contributing to NDACC at IZO are presented (i.e. C2H6, CH4, ClONO2, CO, HCl, HCN, H2CO, HF, HNO3, N2O, NO2, NO, O3, carbonyl sulfide (OCS), and water vapour isotopologues H216O, H218O, and HD16O), reviewing the major accomplishments drawn from these observations. In order to examine the quality and long-term consistency of the IZO FTIR observations, a comparison of those NDACC products for which other high-quality measurement techniques are available at IZO has been performed (i.e. CH4, CO, H2O, NO2, N2O, and O3). This quality assessment was carried out on different timescales to examine what temporal signals are captured by the FTIR records, and to what extent. After 20 years of operation, the IZO NDACC FTIR observations have been found to be very consistent and reliable over time, demonstrating great potential for climate research. Long-term NDACC FTIR data sets, such as IZO, are indispensable tools for the investigation of atmospheric composition trends, multi-year phenomena, and complex climate feedback processes, as well as for the validation of past and present space-based missions and chemistry climate models.

Accurate observations of atmospheric ozone (O3) are essential to monitor in detail its key role in atmospheric chemistry. The present paper examines the performance of different O3 retrieval strategies from FTIR (Fourier transform infrared) spectrometry by using the 20-year time series of the high-resolution solar spectra acquired from 1999 to 2018 at the subtropical Izaña Observatory (IZO, Spain) within NDACC (Network for the Detection of Atmospheric Composition Change). In particular, the effects of two of the most influential factors have been investigated: the inclusion of a simultaneous atmospheric temperature profile fit and the spectral O3 absorption lines used for the retrievals (the broad spectral region of 1000–1005 cm−1 and single micro-windows between 991 and 1014 cm−1). Additionally, the water vapour (H2O) interference in O3 retrievals has been evaluated, with the aim of providing an improved O3 strategy that minimises its impact and, therefore, could be applied at any NDACC FTIR station under different humidity conditions. The theoretical and experimental quality assessments of the different FTIR O3 products (total column (TC) amounts and volume mixing ratio (VMR) profiles) provide consistent results. Combining a simultaneous temperature retrieval with the optimal selection of single O3 micro-windows results in superior FTIR O3 products, with a precision of better than 0.6 %–0.7 % for O3 TCs as compared to coincident NDACC Brewer observations taken as a reference. However, this improvement can only be achieved provided the FTIR spectrometer is properly characterised and stable over time. For unstable instruments, the temperature fit is found to exhibit a strong negative influence on O3 retrievals due to the increase in the cross-interference between the temperature retrieval and instrumental performance (given by the instrumental line shape function and measurement noise), which leads to a worsening of the precision of FTIR O3 TCs of up to 2 %. This cross-interference becomes especially noticeable beyond the upper troposphere/lower stratosphere, as documented theoretically as well as experimentally by comparing FTIR O3 profiles to those measured using electrochemical concentration cell (ECC) sondes within NDACC. Consequently, it should be taken into account for the reliable monitoring of the O3 vertical distribution, especially over long-term timescales.

The reaction of CH 4 with chlorine (Cl) radicals in the atmosphere is associated with an extraordinarily strong isotopic fractionation, where 12 CH 4 reacts about 70 ‰ faster with Cl than 13 CH 4 . Therefore, although the Cl-based sink of CH 4 constitutes only a small contribution to its total removal rate, the uncertainty in this small sink has been identified as one of the two largest uncertainties of isotope-based CH 4 source apportionment at the global scale. The uncertainty arises from the fact that Cl levels in the atmosphere are so low that they cannot be detected directly. One very sensitive indirect method to identify and quantify the CH 4 + Cl reaction in the atmosphere is the detection of the extremely 13 C-depleted reaction product carbon monoxide (CO) from this reaction. This article reviews the concept of this approach, its successful application in the atmosphere, its challenges and opportunities for identifying and quantifying Cl-based removal of CH 4 at the regional and global scale and its potential to detect and evaluate possible attempts to enhance CH 4 removal from the atmosphere.

The reaction of CH4 with chlorine (Cl) radicals in the atmosphere is associated with an extraordinarily strong isotopic fractionation, where 12CH4 reacts about 70 ‰ faster with Cl than 13CH4. Therefore, although the Cl-based sink of CH¬4 constitutes only a small contribution to its total removal rate, the uncertainty in this small sink has been identified as one of the two largest uncertainties of isotope-based CH4 source apportionment at the global scale. The uncertainty arises from the fact that Cl levels in the atmosphere are so low that they cannot be detected directly. One very sensitive indirect method to identify and quantify the CH4 + Cl reaction in the atmosphere is the detection of the extremely 13C-depleted reaction product carbon monoxide (CO) from this reaction. This article reviews the concept of this approach, its successful application in the atmosphere, its challenges and opportunities for identifying and quantifying Cl-based removal of CH4 at the regional and global scale and its potential to detect and evaluate possible attempts to enhance CH4 removal from the atmosphere.

Retrieving high-precision concentrations of atmospheric trace gases from FTIR (Fourier transform infrared) spectrometry requires a precise knowledge of the instrumental performance. In this context, this paper examines the impact on the ozone (O3) retrievals of several approaches used to characterize the instrumental line shape (ILS) function of ground-based FTIR spectrometers within NDACC (Network for the Detection of Atmospheric Composition Change). The analysis has been carried out at the subtropical Izaña Observatory (IZO, Spain) by using the 20-year time series of the high-resolution FTIR solar absorption spectra acquired between 1999 and 2018. The theoretical quality assessment and the comparison to independent O3 observations available at IZO (Brewer O3 total columns and electrochemical concentration cell, ECC, sondes) reveal consistent findings. The inclusion of a simultaneous retrieval of the ILS parameters in the O3 retrieval strategy allows, on the one hand, a rough instrumental characterization to be obtained and, on the other hand, the precision of the FTIR O3 products to be slightly improved. The improvement is of special relevance above the lower stratosphere, where the cross-interference between the O3 vertical distribution and the instrumental performance is more significant. However, it has been found that the simultaneous ILS retrieval leads to a misinterpretation of the O3 variations on daily and seasonal scales. Therefore, in order to ensure the independence of the O3 retrievals and the instrumental response, the optimal approach to deal with the FTIR instrumental characterization is found to be the continuous monitoring of the ILS function by means of independent observations, such as gas cell measurements.