Investigation of strongly enhanced methane Part II: Slow climate feedbacks.

Methane (CH4) is the second most important anthropogenic greenhouse gas and its atmospheric abundance is rising rapidly at the moment (e.g. Nisbet et al., 2019).&#160;We assess the effects of doubled and fivefold present-day (2010) CH4 lower boundary mixing ratios on the basis of sensitivity simulations with the chemistry-climate model EMAC. As a follow-up on Winterstein et al. (2019) we investigate slow adjustments by applying a mixed layer ocean (MLO) model instead of prescribed oceanic conditions. In the simulations with prescribed oceanic conditions, tropospheric temperature changes are largely suppressed, while with MLO tropospheric temperatures adjust to the forcing. In the present study we compare the changes in the MLO sensitivity simulations to the sensitivity simulations with prescribed oceanic conditions (Winterstein et al., 2019). Comparing the responses of these two sets of sensitivity simulations separates rapid adjustments and the effects of slow climate feedbacks associated with tropospheric warming.The chemical interactions in the stratosphere in the MLO set-up (slow adjustments) compare in general well with the results of Winterstein et al. (2019) (rapid adjustments). The increase of stratospheric water vapor is albeit 5 % (15 %) points weaker in the MLO doubling (fivefolding) experiment compared to the doubling (fivefolding) experiment with prescribed oceanic conditions in line with a weaker increase of stratospheric OH. Stronger O3 decrease and CH4 increase in the lowermost tropical stratosphere in the MLO sensitivity simulations compared to the sensitivity simulations with prescribed oceanic conditions indicate a more distinct strengthening of tropical up-welling due to tropospheric warming in the MLO set-up. The MLO simulations also show evidence of a strengthening of the Brewer-Dobson Circulation. When separating the quasi-instantaneous chemically induced O3 response from the O3 response pattern in the MLO set-up, the O3 response to slow climate feedbacks remains. This pattern is consistent with the O3 response to slow climate feedbacks induced by increases of CO2.This first of its kind study shows the climatic impact of strongly enhanced CH4 mixing ratios and how the slow climate response of tropospheric warming potentially damp instantaneous chemical feedbacks.

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Slow feedbacks resulting from strongly enhanced atmospheric methane mixing ratios in a chemistry–climate model with mixed-layer ocean

Atmospheric Chemistry and Physics ◽

10.5194/acp-21-731-2021 ◽

2021 ◽

Vol 21 (2) ◽

pp. 731-754

Author(s):

Laura Stecher ◽

Franziska Winterstein ◽

Martin Dameris ◽

Patrick Jöckel ◽

Michael Ponater ◽

...

Keyword(s):

Water Vapour ◽

Climate Sensitivity ◽

Radiative Forcing ◽

Climate Model ◽

Climate Feedbacks ◽

Mixing Ratios ◽

Mixed Layer Ocean ◽

Radiative Impact ◽

Set Up ◽

Stratospheric Water Vapour

Abstract. In a previous study the quasi-instantaneous chemical impacts (rapid adjustments) of strongly enhanced methane (CH4) mixing ratios have been analysed. However, to quantify the influence of the respective slow climate feedbacks on the chemical composition it is necessary to include the radiation-driven temperature feedback. Therefore, we perform sensitivity simulations with doubled and quintupled present-day (year 2010) CH4 mixing ratios with the chemistry–climate model EMAC (European Centre for Medium-Range Weather Forecasts, Hamburg version – Modular Earth Submodel System (ECHAM/MESSy) Atmospheric Chemistry) and include in a novel set-up a mixed-layer ocean model to account for tropospheric warming. Strong increases in CH4 lead to a reduction in the hydroxyl radical in the troposphere, thereby extending the CH4 lifetime. Slow climate feedbacks counteract this reduction in the hydroxyl radical through increases in tropospheric water vapour and ozone, thereby dampening the extension of CH4 lifetime in comparison with the quasi-instantaneous response. Changes in the stratospheric circulation evolve clearly with the warming of the troposphere. The Brewer–Dobson circulation strengthens, affecting the response of trace gases, such as ozone, water vapour and CH4 in the stratosphere, and also causing stratospheric temperature changes. In the middle and upper stratosphere, the increase in stratospheric water vapour is reduced with respect to the quasi-instantaneous response. We find that this difference cannot be explained by the response of the cold point and the associated water vapour entry values but by a weaker strengthening of the in situ source of water vapour through CH4 oxidation. However, in the lower stratosphere water vapour increases more strongly when tropospheric warming is accounted for, enlarging its overall radiative impact. The response of the stratosphere adjusted temperatures driven by slow climate feedbacks is dominated by these increases in stratospheric water vapour as well as strongly decreased ozone mixing ratios above the tropical tropopause, which result from enhanced tropical upwelling. While rapid radiative adjustments from ozone and stratospheric water vapour make an essential contribution to the effective CH4 radiative forcing, the radiative impact of the respective slow feedbacks is rather moderate. In line with this, the climate sensitivity from CH4 changes in this chemistry–climate model set-up is not significantly different from the climate sensitivity in carbon-dioxide-driven simulations, provided that the CH4 effective radiative forcing includes the rapid adjustments from ozone and stratospheric water vapour changes.

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Investigation of strongly enhanced methane Part I: Chemical feedbacks and rapid adjustments.

10.5194/egusphere-egu2020-9786 ◽

2020 ◽

Author(s):

Franziska Winterstein ◽

Patrick Jöckel ◽

Martin Dameris ◽

Michael Ponater ◽

Fabian Tanalski ◽

...

Keyword(s):

Atmospheric Chemistry ◽

Radiative Forcing ◽

Climate Model ◽

Numerical Study ◽

Stratospheric Ozone ◽

Lower Boundary ◽

Tropospheric Chemistry ◽

Substantial Part ◽

Mixing Ratios ◽

The Impact

Methane (CH4) is the second most important greenhouse gas, which atmospheric concentration is influenced by human activities and currently on a sharp rise. We present a study with numerical simulations using a Chemistry-Climate-Model (CCM), which are performed to assess possible consequences of strongly enhanced CH4 concentrations in the Earth's atmosphere for the climate.Our analysis includes experiments with 2xCH4 and 5xCH4 present day (2010) lower boundary mixing ratios using the CCM EMAC. The simulations are conducted with prescribed oceanic conditions, mimicking present day tropospheric temperatures as its changes are largely suppressed. By doing so we are able to investigate the quasi-instantaneous chemical impact on the atmosphere. We find that the massive increase in CH4 strongly influences the tropospheric chemistry by reducing the OH abundance and thereby extending the tropospheric CH4 lifetime as well as the residence time of other chemical pollutants. The region above the tropopause is impacted by a substantial rise in stratospheric water vapor (SWV). The stratospheric ozone (O3) column increases overall, but SWV induced stratospheric cooling also leads to enhanced ozone depletion in the Antarctic lower stratosphere. Regional&#160; patterns of ozone change are affected by modification of stratospheric dynamics, i.e. increased tropical up-welling and stronger meridional transport&#160; towards the polar regions. We calculate the net radiative impact (RI) of the 2xCH4 experiment to be 0.69 W m-2 and for the 5xCH4 experiment to be 1.79 W m-2. A substantial part of the RI is contributed by chemically induced O3 and SWV changes, in line with previous radiative forcing estimates and is for the first time splitted and spatially asigned to its chemical contributors.This numerical study using a CCM with prescibed oceanic conditions shows the rapid responses to significantly enhanced CH4 mixing ratios, which is the first step towards investigating the impact of possible strong future CH4 emissions on atmospheric chemistry and its feedback on climate.

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Effects of Strongly Enhanced Atmospheric Methane Concentrations in a Fully Coupled Chemistry-Climate Model

10.5194/acp-2020-519 ◽

2020 ◽

Author(s):

Laura Stecher ◽

Franziska Winterstein ◽

Martin Dameris ◽

Patrick Jöckel ◽

Michael Ponater ◽

...

Keyword(s):

Hydroxyl Radical ◽

Water Vapour ◽

Climate Sensitivity ◽

Radiative Forcing ◽

Climate Model ◽

Atmospheric Methane ◽

Climate Feedbacks ◽

Mixing Ratios ◽

Radiative Impact ◽

Stratospheric Water Vapour

Abstract. In a previous study the quasi-instantaneous chemical impacts (rapid adjustments) of strongly enhanced methane (CH4) mixing ratios have been analyzed. However, to quantify the influence of the respective slow climate feedbacks on the chemical composition it is necessary to include the radiation driven temperature feedback. Therefore, we perform sensitivity simulations with doubled and fivefold present-day (year 2010) CH4 mixing ratios with the chemistry-climate model EMAC and include in a novel set-up a mixed layer ocean model to account for tropospheric warming. We find that the slow climate feedbacks counteract the reduction of the hydroxyl radical in the troposphere, which is caused by the strongly enhanced CH4 mixing ratios. Thereby also the resulting prolongation of the tropospheric CH4 lifetime is weakened compared to the quasi-instantaneous response considered previously. Changes in the stratospheric circulation evolve clearly with the warming of the troposphere. The Brewer-Dobson circulation strengthens, affecting the response of trace gases, such as ozone, water vapour and CH4 in the stratosphere, and also causing stratospheric temperature changes. In the middle and upper stratosphere, the increase of stratospheric water vapour is reduced with respect to the quasi-instantaneous response. Weaker increases of the hydroxyl radical cause the chemical depletion of CH4 to be less strongly enhanced and thus the in situ source of stratospheric water vapour as well. However, in the lower stratosphere water vapour increases more strongly when tropospheric warming is accounted for enlarging its overall radiative impact. The response of the stratospheric adjusted temperatures driven by slow climate feedbacks is dominated by these increases of stratospheric water vapour, as well as strongly decreased ozone mixing ratios above the tropical tropopause, which result from enhanced tropical upwelling. While rapid radiative adjustments from ozone and stratospheric water vapour make an essential contribution to the effective CH4 radiative forcing, the radiative impact of the respective slow feedbacks is rather moderate. In line with this, the climate sensitivity from CH4 changes in this chemistry-climate model setup is not significantly different from the climate sensitivity in carbon dioxide-driven simulations, provided that the CH4 effective radiative forcing includes the rapid adjustments from ozone and stratospheric water vapour changes.

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Impacts of Ozone Changes in the Tropopause Layer on Stratospheric Water Vapor

Atmosphere ◽

10.3390/atmos12030291 ◽

2021 ◽

Vol 12 (3) ◽

pp. 291

Author(s):

Jinpeng Lu ◽

Fei Xie ◽

Hongying Tian ◽

Jiali Luo

Keyword(s):

Water Vapor ◽

Ozone Depletion ◽

Climate Model ◽

Global Climate ◽

Stratospheric Water Vapor ◽

Radiative Processes ◽

Low Latitudes ◽

Cold Point ◽

The Impact ◽

Tropopause Temperature

Stratospheric water vapor (SWV) changes play an important role in regulating global climate change, and its variations are controlled by tropopause temperature. This study estimates the impacts of tropopause layer ozone changes on tropopause temperature by radiative process and further influences on lower stratospheric water vapor (LSWV) using the Whole Atmosphere Community Climate Model (WACCM4). It is found that a 10% depletion in global (mid-low and polar latitudes) tropopause layer ozone causes a significant cooling of the tropical cold-point tropopause with a maximum cooling of 0.3 K, and a corresponding reduction in LSWV with a maximum value of 0.06 ppmv. The depletion of tropopause layer ozone at mid-low latitudes results in cooling of the tropical cold-point tropopause by radiative processes and a corresponding LSWV reduction. However, the effect of polar tropopause layer ozone depletion on tropical cold-point tropopause temperature and LSWV is opposite to and weaker than the effect of tropopause layer ozone depletion at mid-low latitudes. Finally, the joint effect of tropopause layer ozone depletion (at mid-low and polar latitudes) causes a negative cold-point tropopause temperature and a decreased tropical LSWV. Conversely, the impact of a 10% increase in global tropopause layer ozone on LSWV is exactly the opposite of the impact of ozone depletion. After 2000, tropopause layer ozone decreased at mid-low latitudes and increased at high latitudes. These tropopause layer ozone changes at different latitudes cause joint cooling in the tropical cold-point tropopause and a reduction in LSWV. Clarifying the impacts of tropopause layer ozone changes on LSWV clearly is important for understanding and predicting SWV changes in the context of future global ozone recovery.

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Effect of the Indo-Pacific Warm Pool on Lower-Stratospheric Water Vapor and Comparison with the Effect of ENSO

Journal of Climate ◽

10.1175/jcli-d-17-0575.1 ◽

2018 ◽

Vol 31 (3) ◽

pp. 929-943 ◽

Cited By ~ 6

Author(s):

Fei Xie ◽

Xin Zhou ◽

Jianping Li ◽

Quanliang Chen ◽

Jiankai Zhang ◽

...

Keyword(s):

Water Vapor ◽

Climate Model ◽

Southern Oscillation ◽

Deep Convection ◽

Warm Pool ◽

Latent Heat Release ◽

Stratospheric Water Vapor ◽

Asymmetric Effects ◽

Pacific Warm Pool ◽

Tropopause Temperature

Abstract Time-slice experiments with the Whole Atmosphere Community Climate Model, version 4 (WACCM4), and composite analysis with satellite observations are used to demonstrate that the Indo-Pacific warm pool (IPWP) can significantly affect lower-stratospheric water vapor. It is found that a warmer IPWP significantly dries the stratospheric water vapor by causing a broad cooling of the tropopause, and vice versa for a colder IPWP. Such imprints in tropopause temperature are driven by a combination of variations in the Brewer–Dobson circulation in the stratosphere and deep convection in the troposphere. Changes in deep convection associated with El Niño–Southern Oscillation (ENSO) reportedly have a small zonal mean effect on lower-stratospheric water vapor for strong zonally asymmetric effects on tropopause temperature. In contrast, IPWP events have zonally uniform imprints on tropopause temperature. This is because equatorial planetary waves forced by latent heat release from deep convection project strongly onto ENSO but weakly onto IPWP events.

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Evaluation of simulated aerosol properties with the aerosol-climate model ECHAM5-HAM using observations from the IMPACT field campaign

Atmospheric Chemistry and Physics ◽

10.5194/acp-10-7709-2010 ◽

2010 ◽

Vol 10 (16) ◽

pp. 7709-7722 ◽

Cited By ~ 20

Author(s):

G.-J. Roelofs ◽

H. ten Brink ◽

A. Kiendler-Scharr ◽

G. de Leeuw ◽

A. Mensah ◽

...

Keyword(s):

Boundary Layer ◽

Climate Model ◽

Lower Boundary ◽

Synoptic Scale ◽

Concentration Gradients ◽

Cloud Properties ◽

Dry Conditions ◽

Strong Exchange ◽

The Impact ◽

Lower Boundary Layer

Abstract. In May 2008, the measurement campaign IMPACT for observation of atmospheric aerosol and cloud properties was conducted in Cabauw, The Netherlands. With a nudged version of the coupled aerosol-climate model ECHAM5-HAM we simulate the size distribution and chemical composition of the aerosol and the associated aerosol optical thickness (AOT) for the campaign period. Synoptic scale meteorology is represented realistically through nudging of the vorticity, the divergence, the temperature and the surface pressure. Simulated concentrations of aerosol sulfate and organics at the surface are generally within a factor of two from observed values. The monthly averaged AOT from the model is 0.33, about 20% larger than observed. For selected periods of the month with relatively dry and moist conditions discrepancies are approximately −30% and +15%, respectively. Discrepancies during the dry period are partly caused by inaccurate representation of boundary layer (BL) dynamics by the model affecting the simulated AOT. The model simulates too strong exchange between the BL and the free troposphere, resulting in weaker concentration gradients at the BL top than observed for aerosol and humidity, while upward mixing from the surface layers into the BL appears to be underestimated. The results indicate that beside aerosol sulfate and organics also aerosol ammonium and nitrate significantly contribute to aerosol water uptake. The simulated day-to-day variability of AOT follows synoptic scale advection of humidity rather than particle concentration. Even for relatively dry conditions AOT appears to be strongly influenced by the diurnal cycle of RH in the lower boundary layer, further enhanced by uptake and release of nitric acid and ammonia by aerosol water.

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Historical greenhouse gas concentrations

10.5194/gmd-2016-169 ◽

2016 ◽

Cited By ~ 6

Author(s):

Malte Meinshausen ◽

Elisabeth Vogel ◽

Alexander Nauels ◽

Katja Lorbacher ◽

Nicolai Meinshausen ◽

...

Keyword(s):

Climate Change ◽

Greenhouse Gas ◽

Radiative Forcing ◽

Sulfur Hexafluoride ◽

Climate Model ◽

Future Climate Change ◽

Large Set ◽

Mixing Ratios ◽

Surface Mixing ◽

Cooling Effects

Abstract. Atmospheric greenhouse gas concentrations are at unprecedented, record-high levels compared to pre-industrial reconstructions over the last 800,000 years. Those elevated greenhouse gas concentrations warm the planet and together with net cooling effects by aerosols, they are the reason of observed climate change over the past 150 years. An accurate representation of those concentrations is hence important to understand and model recent and future climate change. So far, community efforts to create composite datasets with seasonal and latitudinal information have focused on marine boundary layer conditions and recent trends since 1980s. Here, we provide consolidated data sets of historical atmospheric (volume) mixing ratios of 43 greenhouse gases specifically for the purpose of climate model runs. The presented datasets are based on AGAGE and NOAA networks and a large set of literature studies. In contrast to previous intercomparisons, the new datasets are latitudinally resolved, and include seasonality over the period between year 0 to 2014. We assimilate data for CO2, methane (CH4) and nitrous oxide (N2O), 5 chlorofluorocarbons (CFCs), 3 hydrochlorofluorocarbons (HCFCs), 16 hydrofluorocarbons (HFCs), 3 halons, methyl bromide (CH3Br), 3 perfluorocarbons (PFCs), sulfur hexafluoride (SF6), nitrogen triflouride (NF3) and sulfuryl fluoride (SO2F2). We estimate 1850 annual and global mean surface mixing ratios of CO2 at 284.3 ppmv, CH4 at 808.2 ppbv and N2O at 273.0 ppbv and quantify the seasonal and hemispheric gradients of surface mixing ratios. Compared to earlier intercomparisons, the stronger implied radiative forcing in the northern hemisphere winter (due to the latitudinal gradient and seasonality) may help to improve the skill of climate models to reproduce past climate and thereby reduce uncertainty in future projections.

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Modelling marine emissions and atmospheric distributions of halocarbons and DMS: the influence of prescribed water concentration vs. prescribed emissions

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-15-17553-2015 ◽

2015 ◽

Vol 15 (12) ◽

pp. 17553-17598

Author(s):

S. T. Lennartz ◽

G. Krysztofiak-Tong ◽

C. A. Marandino ◽

B.-M. Sinnhuber ◽

S. Tegtmeier ◽

...

Keyword(s):

Wind Speed ◽

Atmospheric Chemistry ◽

Climate Model ◽

Trace Gases ◽

Surface Wind ◽

Water Concentration ◽

Absolute Magnitude ◽

Actual State ◽

Transfer Velocity ◽

Mixing Ratios

Abstract. Marine produced short-lived trace gases such as dibromomethane (CH2Br2), bromoform (CHBr3), methyliodide (CH3I) and dimethylsulfide (DMS) significantly impact tropospheric and stratospheric chemistry. Describing their marine emissions in atmospheric chemistry models as accurately as possible is necessary to quantify their impact on ozone depletion and the Earth's radiative budget. So far, marine emissions of trace gases have mainly been prescribed from emission climatologies, thus lacking the interaction between the actual state of the atmosphere and the ocean. Here we present simulations with the chemistry climate model EMAC with online calculation of emissions based on surface water concentrations, in contrast to directly prescribed emissions. Considering the actual state of the model atmosphere results in a concentration gradient consistent with model real-time conditions at ocean surface and atmosphere, which determine the direction and magnitude of the computed flux. This method has a number of conceptual and practical benefits, as the modelled emission can respond consistently to changes in sea surface temperature, surface wind speed, sea ice cover and especially atmospheric mixing ratio. This online calculation could enhance, dampen or even invert the fluxes (i.e. deposition instead of emissions) of VSLS. We show that differences between prescribing emissions and prescribing concentrations (−28 % for CH2Br2 to +11 % for CHBr3) result mainly from consideration of the actual, time-varying state of the atmosphere. The absolute magnitude of the differences depends mainly on the surface ocean saturation of each particular gas. Comparison to observations from aircraft, ships and ground stations reveals that computing the air–sea flux interactively leads in most of the cases to more accurate atmospheric mixing ratios in the model compared to the computation from prescribed emissions. Calculating emissions online also enables effective testing of different air–sea transfer velocity parameterizations k, which was performed here for eight different parameterizations. The testing of these different k values is of special interest for DMS, as recently published parameterizations derived by direct flux measurements using eddy covariance measurements suggest decreasing k values at high wind speeds or a linear relationship with wind speed. Implementing these parameterizations reduces discrepancies in modelled DMS atmospheric mixing ratios and observations by a factor of 1.5 compared to parameterizations with a quadratic or cubic relationship to wind speed.

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Coral reef-derived dimethyl sulfide and the climatic impact of the loss of coral reefs

10.5194/acp-2020-1054 ◽

2020 ◽

Author(s):

Sonya L. Fiddes ◽

Matthew T. Woodhouse ◽

Todd P. Lane ◽

Robyn Schofield

Keyword(s):

Coral Reef ◽

Coral Reefs ◽

Dimethyl Sulfide ◽

Climate Model ◽

Global Climate Model ◽

Regional Climate ◽

Atmospheric Composition ◽

Aerosol Formation ◽

Climatic Impact ◽

Comparable Amount

Abstract. Dimethyl sulfide (DMS) is a naturally occurring aerosol precursor gas which plays an important role in the global sulfur budget, aerosol formation and climate. While DMS is produced predominantly by phytoplankton, recent observational literature has suggested that corals and their symbionts produce a comparable amount of DMS, which is unaccounted for in models. It has further been hypothesised that the coral reef source of DMS may modulate regional climate. This hypothesis presents a particular concern given the current threat to coral reefs under anthropogenic climate change. In this paper, a global climate model with online chemistry and aerosol is used to explore the influence of coral reef-derived DMS on atmospheric composition and climate. A simple representation of coral reef-derived DMS is developed and added to a common DMS surface water climatology, resulting in an additional DMS flux of 0.3 Tg year−1 S, or 1.7 % of the global flux. By comparing the differences between both nudged and free running ensemble simulations with and without coral reef-derived DMS, the influence of coral reef-derived DMS on regional climate is quantified. In the Maritime Continent-Australian region, where the highest density of coral reefs exist, a small decrease in nucleation and Aitken mode aerosol number concentration and mass is found when coral reef DMS emissions are removed from the system. However, these small responses are found to have no robust effect on regional climate via direct and indirect aerosol effects. This work emphasises the complexities of the aerosol-climate system and the limitations of current modelling capabilities are highlighted, in particular surrounding convective responses to changes in aerosol. In conclusion we find no robust evidence that coral reef-derived DMS influences global and regional climate.

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Chemistry–climate interactions of aerosol nitrate from lightning

Atmospheric Chemistry and Physics ◽

10.5194/acp-17-1125-2017 ◽

2017 ◽

Vol 17 (2) ◽

pp. 1125-1142 ◽

Cited By ~ 8

Author(s):

Holger Tost

Keyword(s):

Climate Model ◽

Statistical Significance ◽

Aerosol Particles ◽

Internal Variability ◽

Aerosol Size Distribution ◽

Upper Troposphere ◽

Uncertainty Range ◽

Mixing Ratios ◽

Microphysical Properties ◽

The Impact

Abstract. Lightning represents one of the dominant emission sources for NOx in the troposphere. The direct release of oxidised nitrogen in the upper troposphere does not only affect ozone formation, but also chemical and microphysical properties of aerosol particles in this region. This study investigates the direct impact of LNOx emissions on upper-tropospheric nitrate using a global chemistry climate model. The simulation results show a substantial influence of the lightning emissions on the mixing ratios of nitrate aerosol in the upper troposphere of more than 50 %. In addition to the impact on nitrate, lightning substantially affects the oxidising capacity of the atmosphere with substantial implications for gas-phase sulfate formation and new particle formation in the upper troposphere. In conjunction with the condensation of nitrates, substantial differences in the aerosol size distribution occur in the upper troposphere as a consequence of lightning. This has implications for the extinction properties of the aerosol particles and for the cloud optical properties. While the extinction is generally slightly enhanced due to the LNOx emissions, the response of the clouds is ambiguous due to compensating effects in both liquid and ice clouds. Resulting shortwave flux perturbations are of ∼ −100 mW m−2 as determined from several sensitivity scenarios, but an uncertainty range of almost 50 % has to be defined due to the large internal variability of the system and the uncertainties in the multitude of involved processes. Despite the clear statistical significance of the influence of lightning on the nitrate concentrations, the robustness of the findings gradually decreases towards the determination of the radiative flux perturbations.

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