Search for: All records

Abstract Atmospheric chemistry plays a crucial role in Earth system models (ESMs), controlling atmospheric composition and radiative balance; it is highly interactive with the physical climate, biogeochemical cycles, and human systems. However, it often imposes computational challenges in an ESM. Here we develop a full troposphere‐stratosphere interactive chemistry module for the US Department of Energy's Energy Exascale Earth System Model (E3SM). We intentionally build a streamlined module based on E3SM version 2 that interacts with other components and maintains all of major chemical and chemistry‐climate feedbacks. The module incorporates a new, highly efficient tracer advection scheme; linearization of stratospheric chemistry; and abridged tropospheric chemical mechanism with 28 reactive tracers. This new model, E3SM‐chem, can readily perform century‐long climate simulations of ozone, methane, and nitrous oxide based on emission scenarios as well as provide hourly budgets for the gas‐phase radicals that drive aerosol chemistry. We evaluate E3SM‐chem with an atmosphere‐only simulation as in the recent climate model intercomparison project (CMIP6) finding results similar to the other CMIP6 models. For the present‐day, E3SM‐chem matches the standard measurement metrics for stratospheric and tropospheric ozone, surface air quality, other key reactive gases like carbon monoxide, and the methane lifetime. Overall, E3SM‐chem maintains the climate fidelity of the baseline model while adding at most 20% to the computational cost of the atmosphere model. Hence, interactive chemistry can be a default configuration for long climate simulations at resolutions of 1° or finer, which is crucial for producing self‐consistent chemistry‐climate feedbacks that alter the climate system. 

Abstract We divide the atmosphere into distinct spheres based on their physical, chemical, and dynamical traits. In deriving chemical budgets and climate trends, which differ across spheres, we need clearly defined boundaries. Our primary spheres are the troposphere and stratosphere (∼99.9% by mass), and the boundary between them is the tropopause. Every global climate‐weather model has one or more methods to calculate the lapse rate tropopause, but these involve subjective choices and are known to fail near the sub‐tropical jets and polar regions. Age‐of‐air tracers clock the effective time‐distance from the tropopause, allowing unambiguous separation of stratosphere from troposphere in the chaotic jet regions. We apply a global model with synthetic tracer e90 (90‐day e‐folding), focusing on ozone and temperature structures about the tropopause using ozone sonde and satellite observations. We calibrate an observation‐consistent tropopause for e90 using tropics‐plus‐midlatitudes and then apply it globally to calculate total tropospheric air‐mass and tropopause ozone values. The tropopause mixing barrier for the current UCI CTM is identified by a transition in the vertical transport gradient to stratospheric values of 15 days km⁻¹, corresponding to an e90 tropopause at 81 ± 2 ppb with a global tropospheric air mass of 82.2 ± 0.3%. The best e90 tropopause based on sonde pressures is 70–80 ppb; but that for ozone is 80–90 ppb, implying that the CTM tropopause ozone values are too large. This approach of calibrating an age‐of‐air tropopause can be readily applied to other models and possibly used with observed age‐of‐air tracers like sulfur hexafluoride. 

Abstract This paper describes the atmospheric component of the US Department of Energy's Energy Exascale Earth System Model (E3SM) version 3. Significant updates have been made to the atmospheric physics compared to earlier versions. Specifically, interactive gas chemistry has been implemented, along with improved representations of aerosols and dust emissions. A new stratiform cloud microphysics scheme more physically treats ice processes and aerosol‐cloud interactions. The deep convection parameterization has been largely improved with sophisticated microphysics for convective clouds, making model convection sensitive to large‐scale dynamics, and incorporating the dynamical and physical effects of organized mesoscale convection. Improvements in aerosol wet removal processes and parameter re‐tuning of key aerosol and cloud processes have improved model aerosol radiative forcing. The model's vertical resolution has increased from 72 to 80 layers with the extra eight layers added in the lower stratosphere to better simulate the Quasi‐Biennial Oscillation. These improvements have enhanced E3SM's capability to couple aerosol, chemistry, and biogeochemistry and reduced some long‐standing biases in simulating tropical variability. Compared to its predecessors, the model shows a much stronger signal for the Madden‐Julian Oscillation, Kelvin waves, mixed Rossby‐gravity waves, and eastward inertia‐gravity waves. Aerosol radiative forcing has been considerably reduced and is now better aligned with community best estimates, leading to significantly improved skill in simulating historical temperature records. Its simulated mean‐state climate is largely comparable to E3SMv2, but with some notable degradation in shortwave cloud radiative effect, precipitable water, and surface wind stress, which will be addressed in future updates. 

Abstract Stratospheric ozone depletion from halocarbons is partly countered by pollution‐driven increases in tropospheric ozone, with transport connecting the two. While recognizing this connection, the ozone assessment's evaluation of observations and processes have often split the chapters at the tropopause boundary. Using a chemistry‐transport model we find that air‐pollution ozone enhancements in the troposphere spill over into the stratosphere at significant rates, that is, 13%–34% of the excess tropospheric burden appears in the lowermost extra‐tropical stratosphere. As we track the anticipated recovery of the observed ozone depletion, we should recognize that two tenths of that recovery may come from the transport of increasing tropospheric ozone into the stratosphere. 

Abstract With increasing global interest in molecular hydrogen to replace fossil fuels, more attention is being paid to potential leakages of hydrogen into the atmosphere and its environmental consequences. Hydrogen is not directly a greenhouse gas, but its chemical reactions change the abundances of the greenhouse gases methane, ozone, and stratospheric water vapor, as well as aerosols. Here, we use a model ensemble of five global atmospheric chemistry models to estimate the 100-year time-horizon Global Warming Potential (GWP100) of hydrogen. We estimate a hydrogen GWP100 of 11.6 ± 2.8 (one standard deviation). The uncertainty range covers soil uptake, photochemical production of hydrogen, the lifetimes of hydrogen and methane, and the hydroxyl radical feedback on methane and hydrogen. The hydrogen-induced changes are robust across the different models. It will be important to keep hydrogen leakages at a minimum to accomplish the benefits of switching to a hydrogen economy. 

Abstract Nitrous oxide (N₂O) is a greenhouse gas and stratospheric ozone‐depleting substance with large and growing anthropogenic emissions. Previous studies identified the influx of N₂O‐depleted air from the stratosphere to partly cause the seasonality in tropospheric N₂O (aN₂O), but other contributions remain unclear. Here, we combine surface fluxes from eight land and four ocean models from phase 2 of the Nitrogen/N₂O Model Intercomparison Project with tropospheric transport modeling to simulate aN₂O at eight remote air sampling sites for modern and pre‐industrial periods. Models show general agreement on the seasonal phasing of zonal‐average N₂O fluxes for most sites, but seasonal peak‐to‐peak amplitudes differ several‐fold across models. The modeled seasonal amplitude of surface aN₂O ranges from 0.25 to 0.80 ppb (interquartile ranges 21%–52% of median) for land, 0.14–0.25 ppb (17%–68%) for ocean, and 0.28–0.77 ppb (23%–52%) for combined flux contributions. The observed seasonal amplitude ranges from 0.34 to 1.08 ppb for these sites. The stratospheric contributions to aN₂O, inferred by the difference between the surface‐troposphere model and observations, show 16%–126% larger amplitudes and minima delayed by ∼1 month compared to Northern Hemisphere site observations. Land fluxes and their seasonal amplitude have increased since the pre‐industrial era and are projected to grow further under anthropogenic activities. Our results demonstrate the increasing importance of land fluxes for aN₂O seasonality. Considering the large model spread, in situ aN₂O observations and atmospheric transport‐chemistry models will provide opportunities for constraining terrestrial and oceanic biosphere models, critical for projecting carbon‐nitrogen cycles under ongoing global warming. 

Abstract. We present gridded surface air quality datasets over South Korea for three key species – ozone (O3), carbon monoxide (CO), and nitrogen oxides (NOx) during the timeframe of the Korea–US Air Quality (KORUS–AQ) mission (May–June 2016). The tenth degree hourly averaged abundances are constructed from the 300+ air quality network sites using inverse distance weighting with simple declustering. Cross–comparing the interpolated fields against the site data that was used to create them reveals high prediction skill for O3 (80 %) throughout South Korea, and moderate skill (60 %) for CO and NOx on average in densely observed regions after individual mean bias corrections. The gridded O3 and CO interpolations predict the NASA DC–8 observations in the planetary boundary layer (PBL) with high skill (80 %) in the Seoul Metropolitan Area (SMA) after subtracting the mean bias. DC–8 NOx observations were much less predictable on account of consistently negative vertical gradients within the PBL. Our gridded products capture the mean and variability of O3 throughout South Korea, and of CO and surface NOx in most site–dense urban centres (SMA, Cheongju, Gwangju, Daegu, Changwon, and Busan). 

The decay of methyl chloroform, a banned ozone-depleting substance, has provided a clear observational metric of mean tropospheric hydroxyl radical (OH) abundance. Almost all current global chemistry models calculate about 15% too much OH and thus too rapid methane loss. Methane is a short-lived climate forcer, critical to achieving global warming targets, and this error affects our model projections of climate change. New observations of water vapor absorption in the ultraviolet region (290 to 350 nanometers) imply reductions in sunlight with key photolysis rates decreasing by 8 to 12% in the near-surface tropical atmosphere. Incorporation of this new mechanism in a chemistry-transport model reduces OH and methane loss by only 4%, but combined with other proposed mechanisms, such as tropospheric halogen chemistry (7%), we may be able to resolve this conundrum. 

The lifetime of tropospheric O3 is difficult to quantify because we model O3 as a secondary pollutant, without direct emissions. For other reactive greenhouse gases like CH4 and N2O, we readily model lifetimes and timescales that include chemical feedbacks based on direct emissions. Here, we devise a set of artificial experiments with a chemistry-transport model where O3 is directly emitted into the atmosphere at a quantified rate. We create 3 primary emission patterns for O3, mimicking secondary production by surface industrial pollution, that by aviation, and primary injection through stratosphere–troposphere exchange (STE). The perturbation lifetimes for these O3 sources includes chemical feedbacks and varies from 6 to 27 days depending on source location and season. Previous studies derived lifetimes around 24 days estimated from the mean odd-oxygen loss frequency. The timescales for decay of excess O3 varies from 10 to 20 days in northern hemisphere summer to 30 to 40 days in northern hemisphere winter. For each season, we identify a single O3 chemical mode applying to all experiments. Understanding how O3 sources accumulate (the lifetime) and disperse (decay timescale) provides some insight into how changes in pollution emissions, climate, and stratospheric O3 depletion over this century will alter tropospheric O3. This work incidentally found 2 distinct mistakes in how we diagnose tropospheric O3, but not how we model it. First, the chemical pattern of an O3 perturbation or decay mode does not resemble our traditional view of the odd-oxygen family of species that includes NO2. Instead, a positive O3 perturbation is accompanied by a decrease in NO2. Second, heretofore we diagnosed the importance of STE flux to tropospheric O3 with a synthetic “tagged” tracer O3S, which had full stratospheric chemistry and linear tropospheric loss based on odd-oxygen loss rates. These O3S studies predicted that about 40% of tropospheric O3 was of stratospheric origin, but our lifetime and decay experiments show clearly that STE fluxes add about 8% to tropospheric O3, providing further evidence that tagged tracers do not work when the tracer is a major species with chemical feedbacks on its loss rates, as shown previously for CH4.