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At least 253 records · Page 14

Multi-Model Assessment of the Factors Driving Stratospheric Ozone Evolution Over the 21st Century

The evolution of stratospheric ozone from 1960 to 2100 is examined in simulations from fourteen chemistry-climate models. There is general agreement among the models at the broadest levels, showing column ozone decreasing at all latitudes from 1960 to around 2000, then increasing at all latitudes over the first half of the 21st century, and latitudinal variations in the rate of increase and date of return to historical values. In the second half of the century, ozone is projected to continue increasing, level off or even decrease depending on the latitude, resulting in variable dates of return to historical values at latitudes where column ozone has declined below those levels. Separation into partial column above and below 20 hPa reveals that these latitudinal differences are almost completely due to differences in the lower stratosphere. At all latitudes, upper stratospheric ozone increases throughout the 21st century and returns to 1960 levels before the end of the century, although there is a spread among the models in dates that ozone returns to historical values. Using multiple linear regression, we find decreasing halogens and increasing greenhouse gases contribute almost equally to increases in the upper stratospheric ozone. In the tropical lower stratosphere an increase in tropical upwelling causes a steady decrease in ozone through the 21st century, and total column ozone does not return to 1960 levels in all models. In contrast, lower stratospheric and total column ozone in middle and high latitudes increases during the 21st century and returns to 1960 levels.

Oman, L. D.↗

Variability of Irreversible Poleward Transport in the Lower Stratosphere

The ascent and descent of the Brewer-Dobson circulation plays a large role in determining the distributions of many constituents in the extratropical lower stratosphere. However, relatively fast, quasi-horizontal transport out of the tropics and polar regions also significantly contribute to determining these distributions. The tropical tape recorder signal assures that there must be outflow from the tropics into the extratropical lower stratosphere. The phase of the quasi-biennial oscillation (QBO) and state of the polar vortex are known to modulate the transport from the tropical and polar regions, respectively. In this study we examine multiple years of ozone distributions in the extratropical lower stratosphere observed by the Aura Microwave Limb Sounder (MLS) and the Aura High Resolution Dynamic Limb Sounder (HIRDLS). The distributions are compared with analyses of irreversible, meridional isentropic transport. We show that there is considerable year-to-year seasonal variability in the amount of irreversible transport from the tropics, which is related to both the phase of the QBO and the state of the polar vortex. The reversibility of the transport is consistent with the number of observed breaking waves. The variability of the atmospheric index of refraction in the lower stratosphere is shown to be significantly correlated with the wave breaking and amount of irreversible transport. Finally, we will show that the seasonal extratropical stratosphere to troposphere transport of ozone can be substantially modulated by the amount of irreversible meridional transport in the lower stratosphere and we investigate how observable these differences are in data of tropospheric ozone.

Olsen, Mark↗

Influence of Aerosol Heating on the Stratospheric Transport of the Mt. Pinatubo Eruption

On June 15th, 1991 the eruption of Mt. Pinatubo (15.1 deg. N, 120.3 Deg. E) in the Philippines injected about 20 Tg of sulfur dioxide in the stratosphere, which was transformed into sulfuric acid aerosol. The large perturbation of the background aerosol caused an increase in temperature in the lower stratosphere of 2-3 K. Even though stratospheric winds climatological]y tend to hinder the air mixing between the two hemispheres, observations have shown that a large part of the SO2 emitted by Mt. Pinatubo have been transported from the Northern to the Southern Hemisphere. We simulate the eruption of Mt. Pinatubo with the Goddard Earth Observing System (GEOS) version 5 global climate model, coupled to the aerosol module GOCART and the stratospheric chemistry module StratChem, to investigate the influence of the eruption of Mt. Pinatubo on the stratospheric transport pattern. We perform two ensembles of simulations: the first ensemble consists of runs without coupling between aerosol and radiation. In these simulations the plume of aerosols is treated as a passive tracer and the atmosphere is unperturbed. In the second ensemble of simulations aerosols and radiation are coupled. We show that the set of runs with interactive aerosol produces a larger cross-equatorial transport of the Pinatubo cloud. In our simulations the local heating perturbation caused by the sudden injection of volcanic aerosol changes the pattern of the stratospheric winds causing more intrusion of air from the Northern into the Southern Hemisphere. Furthermore, we perform simulations changing the injection height of the cloud, and study the transport of the plume resulting from the different scenarios. Comparisons of model results with SAGE II and AVHRR satellite observations will be shown.

Aquila, Valentina↗

Influence of an Internally-Generated QBO on Modeled Stratospheric Dynamics and Ozone

A GEOS V2 CCM simulation with an internally generated quasi-biennial oscillation (QBO) signal is compared to an otherwise identical simulation without a QBO. In a present-day climate, inclusion of the modeled QBO makes a significant difference to stratospheric dynamics and ozone throughout the year. The QBO enhances variability in the tropics, as expected, but also in the polar stratosphere in some seasons. The modeled QBO also affects the mean stratospheric climate. Because tropical zonal winds in the baseline simulation are generally easterly, there is a relative increase in zonal wind magnitudes in tropical lower and middle stratosphere in the QBO simulation. Extra-tropical differences between the QBO and 'no QBO' simulations thus reflect a bias toward the westerly phase of the QBO: a relative strengthening and poleward shifting the polar stratospheric jets, and a reduction in Arctic lower stratospheric ozone.

Hurwitz, M. M.↗

Multimodel Assessment of the Factors Driving Stratospheric Ozone Evolution over the 21st Century

The evolution of stratospheric ozone from 1960 to 2100 is examined in simulations from 14 chemistry-climate models, driven by prescribed levels of halogens and greenhouse gases. There is general agreement among the models that total column ozone reached a minimum around year 2000 at all latitudes, projected to be followed by an increase over the first half of the 21st century. In the second half of the 21st century, ozone is projected to continue increasing, level off, or even decrease depending on the latitude. Separation into partial columns above and below 20 hPa reveals that these latitudinal differences are almost completely caused by differences in the model projections of ozone in the lower stratosphere. At all latitudes, upper stratospheric ozone increases throughout the 21st century and is projected to return to 1960 levels well before the end of the century, although there is a spread among models in the dates that ozone returns to specific historical values. We find decreasing halogens and declining upper atmospheric temperatures, driven by increasing greenhouse gases, contribute almost equally to increases in upper stratospheric ozone. In the tropical lower stratosphere, an increase in upwelling causes a steady decrease in ozone through the 21st century, and total column ozone does not return to 1960 levels in most of the models. In contrast, lower stratospheric and total column ozone in middle and high latitudes increases during the 21st century, returning to 1960 levels well before the end of the century in most models.

Oman, L. D.↗

Sensitivity of Stratospheric Geoengineering with Black Carbon to Aerosol Size and Altitude of Injection

Simulations of stratospheric geoengineering with black carbon (BC) aerosols using a general circulation model with fixed sea surface temperatures show that the climate effects strongly depend on aerosol size and altitude of injection. 1 Tg BC/a injected into the lower stratosphere would cause little surface cooling for large radii but a large amount of surface cooling for small radii and stratospheric warming of over 60 C. With the exception of small particles, increasing the altitude of injection increases surface cooling and stratospheric warming. Stratospheric warming causes global ozone loss by up to 50% in the small radius case. The Antarctic shows less ozone loss due to reduction of polar stratospheric clouds, but strong circumpolar winds would enhance the Arctic ozone hole. Using diesel fuel to produce the aerosols is likely prohibitively expensive and infeasible. Although studying an absorbing aerosol is a useful counterpart to previous studies involving sulfate aerosols, black carbon geoengineering likely carries too many risks to make it a viable option for deployment.

Kravitz, Ben↗

Temperature Trends in the Tropical Upper Troposphere and Lower Stratosphere: Connections with Sea Surface Temperatures and Implications for Water Vapor and Ozone

Satellite observations and chemistry-climate model experiments are used to understand the zonal structure of tropical lower stratospheric temperature, water vapor, and ozone trends. The warming in the tropical upper troposphere over the past 30 years is strongest near the Indo-Pacific warm pool, while the warming trend in the western and central Pacific is much weaker. In the lower stratosphere, these trends are reversed: the historical cooling trend is strongest over the Indo-Pacific warm pool and is weakest in the western and central Pacific. These zonal variations are stronger than the zonal-mean response in boreal winter. Targeted experiments with a chemistry-climate model are used to demonstrate that sea surface temperature (hereafter SST) trends are driving the zonal asymmetry in upper tropospheric and lower stratospheric tropical temperature trends. Warming SSTs in the Indian Ocean and in the warm pool region have led to enhanced moist heating in the upper troposphere, and in turn to a Gill-like response that extends into the lower stratosphere. The anomalous circulation has led to zonal structure in the ozone and water vapor trends near the tropopause, and subsequently to less water vapor entering the stratosphere. The radiative impact of these changes in trace gases is smaller than the direct impact of the moist heating. Projected future SSTs appear to drive a temperature and water vapor response whose zonal structure is similar to the historical response. In the lower stratosphere, the changes in water vapor and temperature due to projected future SSTs are of similar strength to, though slightly weaker than, that due directly to projected future CO2, ozone, and methane.

water vapor↗

Methane as a Diagnostic Tracer of Changes in the Brewer-Dobson Circulation of the Stratosphere

This study makes use of time series of methane (CH4/ data from the Halogen Occultation Experiment (HALOE) to detect whether there were any statistically significant changes of the Brewer-Dobson circulation (BDC) within the stratosphere during 1992-2005. The HALOE CH4 profiles are in terms of mixing ratio versus pressure altitude and are binned into latitude zones within the Southern Hemisphere and the Northern Hemisphere. Their separate time series are then analyzed using multiple linear regression (MLR) techniques. The CH4 trend terms for the Northern Hemisphere are significant and positive at 10 N from 50 to 7 hPa and larger than the tropospheric CH4 trends of about 3%decade(exp -1) from 20 to 7 hPa. At 60 N the trends are clearly negative from 20 to 7 hPa. Their combined trends indicate an acceleration of the BDC in the middle stratosphere of the Northern Hemisphere during those years, most likely due to changes from the effects of wave activity. No similar significant BDC acceleration is found for the Southern Hemisphere. Trends from HALOE H2O are analyzed for consistency. Their mutual trends with CH4 are anti-correlated qualitatively in the middle and upper stratosphere, where CH4 is chemically oxidized to H2O. Conversely, their mutual trends in the lower stratosphere are dominated by their trends upon entry to the tropical stratosphere. Time series residuals for CH4 in the lower mesosphere also exhibit structures that are anti-correlated in some instances with those of the tracer-like species HCl. Their occasional aperiodic structures indicate the effects of transport following episodic, wintertime wave activity. It is concluded that observed multi-year, zonally averaged distributions of CH4 can be used to diagnose major instances of wave-induced transport in the middle atmosphere and to detect changes in the stratospheric BDC.

Remsberg, E. E.↗

SPARC's Stratospheric Sulfur and its Role in Climate Activity (SSiRC)

The stratospheric aerosol layer is a key component in the climate system. It affects the radiative balance of the atmosphere directly through interactions with solar and terrestrial radiation, and indirectly through its effect on stratospheric ozone. Because the stratospheric aerosol layer is prescribed in many climate models and Chemistry-Climate Models (CCMs), model simulations of future atmospheric conditions and climate generally do not account for the interaction between the aerosol-sulfur cycle and changes in the climate system. The present understanding of how the stratospheric aerosol layer may be affected by future climate change and how the stratospheric aerosol layer may drive climate change is, therefore, very limited. The purposes of SSiRC (Stratospheric Sulfur and its Role in Climate) include: (i) providing a coordinating structure for the various individual activities already underway in different research centers; (ii) encouraging and supporting new instrumentation and measurements of sulfur containing compounds, such as COS, DMS, and non-volcanic SO2 in the UT/LS globally; and (iii) initiating new model/data inter-comparisons. SSiRC is developing collaborations with a number of other SPARC activities including CCMI and ACAM. This presentation will highlight the scientific goals of this project and on-going activities and propose potential interactions between SSiRC and ACAM.

Thomason, Larry↗

Hemispheric Differences in Tropical Lower Stratospheric Transport and Tracers Annual Cycle

Transport of long-lived tracers (such as O, CO, and N O) in the lower stratosphere largely determines the composition of the entire stratosphere. Stratospheric transport includes the mean residual circulation (with air rising in the tropics and sinking in the polar and middle latitudes), plus two-way isentropic (quasi-horizontal) mixing by eddies. However, the relative importance of two transport components remains uncertain. Previous studies quantified the relative role of these processes based on tropics-wide average characteristics under common assumption of well-mixed tropics. However, multiple instruments provide us with evidence that show significant differences in the seasonal cycle of ozone between the Northern (0-20N) and Southern (0-20S) tropical (NT and ST respectively) lower stratosphere. In this study we investigate these differences in tracer seasonality and quantify transport processes affecting tracers annual cycle amplitude using simulations from Goddard Earth Observing System Chemistry Climate Model (GEOSCCM) and Whole Atmosphere Community Climate Model (WACCM) and compare them to observations from the Microwave Limb Sounder (MLS) on the Aura satellite. We detect the observed contrast between the ST and NT in GEOSCCM and WACCM: annual cycle in ozone and other chemical tracers is larger in the NT than in the ST but opposite is true for the annual cycle in vertical advection. Ozone budgets in the models, analyzed based on the Transformed Eulerian Mean (TEM) framework, demonstrate a major role of quasi-horizontal mixing vertical advection in determining the NTST ozone distribution and behavior. Analysis of zonal variations in the NT and ST ozone annual cycles further suggests important role of North American and Asian Summer Monsoons (associated with strong isentropic mixing) on the lower stratospheric ozone in the NT. Furthermore, multi model comparison shows that most CCMs reproduce the observed characteristic of ozone annual cycle quite well. Thus, latitudinal variations within the tropics have to be considered in order to understand the balance between upwelling and quasi- horizontal mixing in the tropical lower stratosphere and the paradigm of well mixed tropics has to be reconsidered.

Chemistry-Climate Models↗

Wildfire-driven Thunderstorms Cause a Volcano-Like Stratospheric Injection of Smoke

Intense heating by wildfires can generate deep, smoke-infused thunderstorms, known as pyrocumulonimbus (pyroCb), which can release a large quantity of smoke particles above jet aircraft cruising altitudes. Injections of pyroCb smoke into the lower stratosphere have gained increasing attention over the past 15 years due to the rapid proliferation of satellite remote sensing tools. Impacts from volcanic eruptions and other troposphere-to-stratosphere exchange processes on stratospheric radiative and chemical equilibrium are well recognized and monitored. However, the role of pyroCb smoke in the climate system has yet to be acknowledged. Here, we show that the mass of smoke aerosol particles injected into the lower stratosphere from five near-simultaneous intense pyroCbs occurring in western North America on 12 August 2017 was comparable to that of a moderate volcanic eruption, and an order of magnitude larger than previous benchmarks for extreme pyroCb activity. The resulting stratospheric plume encircled the Northern Hemisphere over several months. By characterizing this event, we conclude that pyroCb activity, considered as either large singular events, or a full fire season inventory, significantly perturb the lower stratosphere in a manner comparable with infrequent volcanic intrusions.

Pyrocumulonimbus (pyroCb)↗

Joint Assimilation of the Aura Microwave Limb Sounder and Ozone Mapping and Profiler Suite Limb Profiler Data: Towards a Reanalysis of Stratospheric Ozone for Trend Studies

The future trajectory of the stratospheric ozone recovery will be sensitive to greenhouse gas concentrations through thermal control of chemical loss and via stratospheric circulation changes. The latter in particular is subject to considerable uncertainty meriting continuing monitoring of the evolution of ozone throughout the depth of the stratosphere. Atmospheric reanalyses utilize the data assimilation methodology to obtain comprehensive representations of the state of the atmosphere, including its composition, on multidecadal scales by combining diverse measurements from satellite-borne and conventional data sources. Systematic biases among these various data types pose a challenge for assimilation by introducing spurious discontinuities that affect the utility of reanalyses for studies of long-term variability and trends.In this presentation we will outline an approach, developed at NASA's Global Modeling and Assimilation Office (GMAO), that allows joint assimilation of stratospheric ozone profiles from the Microwave Limb Sounder (MLS) on EOS Aura and the Ozone Mapping and Profiler Suite Limb Profiler (OMPS-LP) currently flying on the Suomi-NPP satellite with future missions projected into the 2030s. We will demonstrate that a simple offline correction significantly reduces biases between MLS and OMPS-LP ozone data providing a strategy for generating a long-term vertically resolved homogenized representation of stratospheric ozone in future reanalyses. One novel element of our approach compared to previous GMAO reanalysis is the use of a version of the Goddard Earth Observing System model with full stratospheric chemistry. We will show selected comparisons of MLS and OMPS-LP assimilation experiments with independent ozonesonde and satellite data as well as two examples of process-based evaluation focused on the 2016 QBO disruption and Arctic winter ozone loss focusing on the relative performance of the MLS and OMPS-LP analyses.

Wargan, K.↗

Evaluation of the Stratospheric and Tropospheric Bromine Burden over Fairbanks, Alaska Based on Column Retrievals of Bromine Monoxide

In spring 2011, columns of bromine monoxide (BrO) were retrieved over Fairbanks, Alaska using a ground-based multifunction differential optical absorption spectroscopy (MFDOAS) instrument. MFDOAS vertical column BrO is consistently lower than retrievals from the satellite-based Ozone Monitoring Instrument (OMI), with a relative bias of 20 ± 14%. Numerous tropical-based studies suggest that 5 ± 2 ppt of bromine from very short-lived substances (VSLS) reaches the stratosphere. We evaluate upper limits on the contribution of VSLS to stratospheric bromine by treating the column retrievals of BrO as purely stratospheric and modeling the ratio of BrO to total inorganic bromine. The OMI and MFDOAS retrievals respectively present 8 and 5 ppt upper limits on the stratospheric injection of VSLS, and kinetic uncertainties in the daytime partitioning of bromine species decrease both values by ~1.6 ppt. The OMI-based estimate is in agreement with the 5 ppt tropical-based value for stratospheric injection of VSLS if the tropospheric column of BrO is 1.5 × 10(exp 13) molecules/cu. cm over Fairbanks, which is within the range of uncertainty of a second ground-based instrument that monitored tropospheric BrO during the campaign. Because our ground-based instruments detected no BrO near the surface, this value for tropospheric BrO would originate from the free troposphere and is in agreement with previous retrievals of background tropospheric BrO. Our calculations of tropospheric BrO over Fairbanks are most sensitive to uncertainties in the stratospheric loading of VSLS, followed by the difference between the OMI and MFDOAS retrievals of BrO.

Pamela A. Wales↗

From the Upper Troposphere Through the Stratosphere: How Satellite Measurements Help Us Decode the Past to Better Project the Future

Decades of observations of key chemical species are allowing us to more fully understand processes important to transport and composition from the upper troposphere through the stratosphere. This talk will focus on a few examples and how they are informing our understanding of variability, trends, and future projections. The growth of the Antarctic ozone hole (late 1970s – mid 1990s) caused a dynamical perturbation to the Southern Hemisphere stratospheric circulation visible in ozone, one of our longest and best observed chemical constituents, and illustrates the connection between chemical change and the coupled radiative and dynamical response that challenges chemistry-climate models (CCMs). The quasi-biennial oscillation (QBO) is the dominant mode of interannual variability in the tropical stratosphere, however its impacts on stratospheric circulation and composition can be traced globally. The QBOs timing with respect to the seasonal cycle in each hemisphere is significant in understanding its impact on up to decadal scale variability. The El Nino Southern Oscillation (ENSO), which dominates tropical tropospheric interannual variability, also affects the stratosphere and its influence is visible in our growing record of tropospheric and stratospheric composition measurements. I will discuss how our knowledge of response has grown and how representation of these observed responses in CCMs is key both to understanding recent trends and to reducing uncertainty in future changes of composition.

Luke David Oman↗

Residual Temperature Bias Effects in Stratospheric Species Distributions from LIMS

The Nimbus 7 Limb Infrared Monitor of theStratosphere (LIMS) instrument operated from 25 Octo-ber 1978 through 28 May 1979. Its version 6 (V6) profileswere processed and archived in 2002. We present severaldiagnostic examples of the quality of the V6 stratospheric species distributions based on their level 3 zonal Fourier co-efficient products. In particular, we show that there are smalldifferences in the ascending (A) minus descending (D) or-bital temperature–pressure orT(p) profiles (theirA−Dval-ues) that affect (A−D) species values. SystematicA−Dbi-ases inT(p) can arise from small radiance biases and/or fromviewing anomalies along orbits. There can also be (A−D)differences inT(p) due to not resolving and correcting forall of the atmospheric temperature gradient along LIMS tan-gent view-paths. An error inT(p) affects species retrievalsthrough (1) the Planck blackbody function in forward calcu-lations of limb radiance that are part of the iterative retrievalalgorithm of LIMS, and (2) the registration of the measuredLIMS species radiance profiles in pressure altitude, mainlyfor the lower stratosphere. There are clearA−Ddifferencesfor ozone, H2O, and HNO3but not for NO2. Percentage differences are larger in the lower stratosphere for ozone andH2O because those species are optically thick. We evaluateV6 ozone profile biases in the upper stratosphere with the aid of comparisons against a monthly climatology of UV–ozone soundings from rocketsondes. We also provide resultsof time series analyses of V6 ozone, H2O, and potential vor-ticity for the middle stratosphere to show that their average(A+D) V6 level 3 products provide a clear picture of the evolution of those tracers during Northern Hemisphere win-ter. We recommend that researchers use the average V6 level3 product for their science studies of stratospheric ozone andH2O, while keeping in mind that there are uncorrected non-local thermodynamic equilibrium effects in daytime ozone inthe lower mesosphere and in daytime H2O in the uppermoststratosphere. We also point out that the present-day Soundingof the Atmosphere using Broadband Emission Radiometry(SABER) experiment provides measurements and retrievalsof temperature and ozone that are nearly free of anomalousdiurnal variations and of effects from gradients at low and middle latitudes.

Ellis Remsberg↗

Large Anomalies in Lower Stratospheric Water Vapor and Ice During the 2015–2016 El Niño

The strong and unusual El Niño of 2015-2016 produced a remarkable perturbation to the hydrologic budget of the tropical tropopause layer (14-19 km). This region regulates stratospheric water vapor, which has a direct radiative impact on surface temperatures. To first order, the coldest tropical tropopause temperature regulates the amount of water vapor entering the stratosphere by controlling the amount of dehydration in the rising air. Here we show that tropical convective cloud ice and associated cirrus evaporating at unusually high altitudes might also have a role in stratospheric hydration. The 2015-2016 El Niño produced decadal record water vapor amounts in the tropical Western Pacific, coincident with warm tropopause temperature anomalies. In the Central Pacific, convective cloud ice was observed 2 km above the anomalously cold tropopause. A trajectory-based dehydration model based on two reanalysis temperature and wind fields can account for only about 0.5-0.6 ppmv of the ~0.9 ppmv tropical lower stratospheric moistening observed during this event. This suggests that unresolved convective dynamics and/or associated sublimation of lofted ice particles also contributed to lower stratospheric moistening. These observations suggest that convective moistening could contribute to future climate change-induced stratospheric water vapor increases.

Atmospheric chemistry↗

Tracking the Hunga Tonga-Hunga Ha’apai Eruption Stratospheric Aerosol and Trace Gas Plumes Using Machine Learning

The Hunga Tonga-Hunga Ha’apai (HTHH) submarine volcano had an explosive eruption phase on January 15, 2022, that thrusted ash, gases, and water vapor through the troposphere and into the stratosphere. The stratospheric volcanic plume included aerosol precursor gases such as SO2 and H2S as well as anomalously high water vapor concentrations due to the submarine oceanic origin. With these atmospheric constituents, the sulfuric gases and water vapor formed sulfate (SO4) particles via gas-to-particle reactions and these aerosols likely increased in size due to hygroscopic growth within anomalously humid regions. Strong easterlies and gravity waves propagated the volcanic impacts throughout the stratosphere. Orbital and suborbital passive sensor retrievals detected changes in the aerosol and trace gas characteristics within the atmospheric column for cloud-free regions over the southern hemisphere. While the CALIPSO lidar can detect aerosol layers in the stratosphere, passive sensors such as MODIS retrieved the total column aerosol abundance and characteristics. Previous studies used manual tracking methods to determine volcanic plume positions and compared them to ground observations. In this study, we examine the machine learning (ML) approaches including segmentation, object detection, and object tracking to identify and track aerosol and trace gas plumes using orbital and suborbital sensor data. This ML implementation strives to provide a more systematic approach to separate total column effects from those of the stratosphere. Similar ML tracking may be useful for stratospheric impact events observed historically by CALIPSO and in the future with EarthCare and the Atmosphere Observing System (AOS) lidar-capable missions.

Rhys Leahy↗

Solar FTIR Measurements of NOx Vertical Distributions – Part 2: Experiment-Based Scaling Factors Describing the Daytime Variation in Stratospheric NOx

Long-term experimental stratospheric NO2 and NO partial columns measured by means of solar Fourier-transform infrared (FTIR) spectrometry at Zugspitze (47.42° N, 10.98° E; 2964 m a.s.l.), Germany, were used to create a set of experiment-based monthly scaling factors (SFexp). The underlying data set is published in a companion paper (Nürnberg et al., 2024) and comprises over 25 years of measurements depicting the daytime variability of stratospheric NO2 and NO partial columns with respect to local solar time (LST). In accordance with simulation-based scaling factors recently published by Strode et al. (2022), we created SFexp normalized to SZA =72° for NO2 and NO for every month of the year as a function of solar zenith angle (SZA). Apart from a boundary value problem at minimum SZA values originating from averaging over different times of the month, the obtained scaling factors SFexp(NO2) and SFexp(NO) as a function of SZA represent the daytime behavior already shown in model simulations and experiments in the literature very well. This shows a well-pronounced increase in the NO2 and NO stratospheric partial column with the time of the day and a flattening of this increase after noon. In addition to the discussion of SFexp, we validate the simulation-based scaling factors SFsim(NO2) (Strode et al., 2022) and present simulation-based scaling factors for NO SFsim(NO). The simulation-based scaling factors show excellent agreement with the experiment-based ones; i.e., for NO2 and NO the mean value of the modulus between the experiment and simulation over all SZAs and months is only 0.02 %. We show that recently used model simulations can describe the real behavior of nitrogen oxide (NOx) variability in the stratosphere very well. Furthermore, we conclude that ground-based FTIR measurements can be used for validation of the output of photochemistry models and for creating experiment-based data sets describing the daytime stratospheric NOx variability as a function of SZA. This is a contribution to improved satellite validation and a better understanding of stratospheric photochemistry.

FTIR, nitrogen oxides, diurnal variability↗