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DOE OSTI2022

PNNL Sequim Campus Radionuclide Air Emissions Report for Calendar Year 2021

The U.S. Department of Energy Office of Science (DOE-SC) Pacific Northwest Site Office has oversight and stewardship duties associated with the Pacific Northwest National Laboratory Sequim Campus. Some research projects have the potential to emit low levels of radioactive materials. This report is prepared to document compliance with the Code of Federal Regulation, Title 40, Protection of the Environment, Part 61, National Emission Standards for Hazardous Air Pollutants, Subpart H, “National Emission Standards for Emissions of Radionuclides Other than Radon from Department of Energy Facilities” and Washington Administrative Code Chapter 246-247, "Radiation Protection–Air Emissions." Compliance is indicated by comparing the estimated effective dose equivalent (EDE) to the maximally exposed individual (MEI) member of the public with the 10 millirem per year (mrem/yr) U.S. Environmental Protection Agency (EPA) standard. The PNNL Sequim Campus has only fugitive emissions sources. Despite the fact that the regulations are intended for application to point source emissions, fugitive emissions are included with regard to complying with the EPA standard. The EDE to the Campus MEI due to routine operations in 2021 was 5.4E-05 mrem (5.4E-07 mSv). No non-routine emissions occurred in 2021. The Sequim Campus is in compliance with the federal and state 10 mrem/yr standard.

40 CFR 61 Subpart H↗

DOE OSTI2023

PNNL-Sequim Campus Radionuclide Air Emissions Report for Calendar Year 2022

The U.S. Department of Energy Office of Science (DOE-SC) Pacific Northwest Site Office has oversight and stewardship duties associated with the Pacific Northwest National Laboratory Sequim Campus. Some research projects have the potential to emit low levels of radioactive materials. This report is prepared to document compliance with the Code of Federal Regulation, Title 40, Protection of the Environment, Part 61, National Emission Standards for Hazardous Air Pollutants, Subpart H, “National Emission Standards for Emissions of Radionuclides Other than Radon from Department of Energy Facilities” and Washington Administrative Code Chapter 246-247, "Radiation Protection–Air Emissions." Compliance is indicated by comparing the estimated effective dose equivalent (EDE) to the maximally exposed individual (MEI) member of the public with the 10 millirem per year (mrem/yr) U.S. Environmental Protection Agency (EPA) standard. The PNNL-Sequim Campus has only fugitive emissions sources. Despite the fact that the regulations are intended for application to point source emissions, fugitive emissions are included with regard to complying with the EPA standard. The EDE to the Campus MEI due to routine operations in 2022 was 7.5E-07 mrem (7.5E-09 mSv). No non-routine emissions occurred in 2022. The PNNL-Sequim Campus is in compliance with the federal and state 10 mrem/yr standard.

40 CFR 61 Subpart H↗

DOE OSTI2025

PNNL-Richland Campus Radionuclide Air Emissions Report for Calendar Year 2024

This report documents radionuclide air emissions that result in the 2024 highest effective dose equivalent (EDE) to an offsite member of the public, referred to as the maximally exposed individual (MEI). The report has been prepared in compliance with the Code of Federal Regulations, Title 40, Protection of the Environment, Part 61, National Emission Standards for Hazardous Air Pollutants, Subpart H, “National Emission Standards for Emissions of Radionuclides Other than Radon from Department of Energy Facilities” and Washington Administrative Code Chapter 246-247, “Radiation Protection–Air Emissions.” The total dose to the MEI from all PNNL-Richland campus radionuclide emissions in 2024, including fugitive emissions and radon, is 1.3E-05 mrem (1.3E-07 mSv) EDE, or 100,000 times less than the federal and state standard of 10 mrem/yr, with which the PNNL Richland campus is in compliance. The dose attributable to radon emissions is 4.1E-10 mrem (4.1E-12 mSv) EDE.

40 CFR 61 Subpart H↗

DOE OSTI2026

PNNL Richland Campus Radionuclide Air Emissions Report for Calendar Year 2025

This report documents radionuclide air emissions that result in the 2025 highest effective dose equivalent (EDE) to an offsite member of the public, referred to as the maximally exposed individual (MEI). The report has been prepared in compliance with the Code of Federal Regulations, Title 40, Protection of the Environment, Part 61, National Emission Standards for Hazardous Air Pollutants, Subpart H, “National Emission Standards for Emissions of Radionuclides Other than Radon from Department of Energy Facilities” and Washington Administrative Code Chapter 246-247, “Radiation Protection–Air Emissions.” The total dose to the MEI from all PNNL Richland Campus radionuclide emissions in 2025, including fugitive emissions and radon, is 1.8E-05 mrem (1.8E-07 mSv) EDE, or more than 100,000 times less than the federal and state standard of 10 mrem/yr, with which the PNNL Richland Campus is in compliance. The dose attributable to radon emissions is 1.5E-13 mrem (1.5E-15 mSv) EDE.

40 CFR 61 Subpart H↗

DOE OSTI2022

A Time-Varying Model for Predicting Formaldehyde Emission Rates in Homes

Recent studies have succeeded in relating emissions of various volatile organic compounds to material mass diffusion transfer using detailed empirical characteristics of each of the individual emitting materials. While significant, the resulting models are often scenario specific and/or require a host of individual component parameters to estimate emission rates. This study developed an approach to estimate aggregated emissions rates based on a wide number of field measurements. We used a multi-parameter regression model based on previous mass transfer models to predict formaldehyde emission rate for a whole dwelling using field-measured, time-resolved formaldehyde concentrations, air exchange rates, and indoor environmental parameters in 63 California single-family houses built between 2011 and 2017. The resulting model provides time-varying formaldehyde emission rates, normalized by floor area, for each study home, assuming a well-mixed mass balance transport model of the home, and a well-mixed layer transport model of indoor surfaces. The surface layer model asserts an equilibrium concentration within the surface layer of the emitted materials that is a function of temperature and RH; the dwelling ventilation rate serves as a surrogate for indoor concentration. We also developed a more generic emission model that is suitable for broad prediction of emission for a population of buildings. This model is also based on measurements aggregated from 27 homes from the same study. We showed that errors in predicting household formaldehyde concentrations using this approach were substantially less than those using a traditional constant emission rate model, despite requiring less unique building information.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Utilizing Earth Observations of Soil Freeze/Thaw Data and Atmospheric Concentrations to Estimate Cold Season Methane Emissions in the Northern High Latitudes

The northern wetland methane emission estimates have large uncertainties. Inversion models are a qualified method to estimate the methane fluxes and emissions in northern latitudes but when atmospheric observations are sparse, the models are only as good as their a priori estimates. Thus, improving a priori estimates is a competent way to reduce uncertainties and enhance emission estimates in the sparsely sampled regions. Here, we use a novel way to integrate remote sensing soil freeze/thaw (F/T) status from SMOS satellite to better capture the seasonality of methane emissions in the northern high latitude. The SMOS F/T data provide daily information of soil freezing state in the northern latitudes, and in this study, the data is used to define the cold season in the high latitudes and, thus, improve our knowledge of the seasonal cycle of biospheric methane fluxes. The SMOS F/T data is implemented to LPX-Bern DYPTOP model estimates and the modified fluxes are used as a biospheric a priori in the inversion model CarbonTracker Europe-CH 4 . The implementation of the SMOS F/T soil state is shown to be beneficial in improving the inversion model’s cold season biospheric flux estimates. Our results show that cold season biospheric CH4 emissions in northern high latitudes are approximately 0.60 Tg lower than previously estimated, which corresponds to 17% reduction in the cold season biospheric emissions. This reduction is partly compensated by increased anthropogenic emissions in the same area (0.23 Tg), and the results also indicates that the anthropogenic emissions could have even larger contribution in cold season than estimated here.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2016

PREDICTION OF FORBIDDEN ULTRAVIOLET AND VISIBLE EMISSIONS IN COMET 67P/CHURYUMOV–GERASIMENKO

Remote observation of spectroscopic emissions is a potential tool for the identification and quantification of various species in comets. The CO Cameron band (to trace CO{sub 2}) and atomic oxygen emissions (to trace H{sub 2}O and/or CO{sub 2}, CO) have been used to probe neutral composition in the cometary coma. Using a coupled-chemistry-emission model, various excitation processes controlling the CO Cameron band and different atomic oxygen and atomic carbon emissions have been modeled in comet 67P/Churyumov–Gerasimenko at 1.29 AU (perihelion) and at 3 AU heliocentric distances, which is being explored by ESA's Rosetta mission. The intensities of the CO Cameron band, atomic oxygen, and atomic carbon emission lines as a function of projected distance are calculated for different CO and CO{sub 2} volume mixing ratios relative to water. Contributions of different excitation processes controlling these emissions are quantified. We assess how CO{sub 2} and/or CO volume mixing ratios with respect to H{sub 2}O can be derived based on the observed intensities of the CO Cameron band, atomic oxygen, and atomic carbon emission lines. The results presented in this work serve as baseline calculations to understand the behavior of low out-gassing cometary coma and compare them with the higher gas production rate cases (e.g., comet Halley). Quantitative analysis of different excitation processes governing the spectroscopic emissions is essential to study the chemistry of inner coma and to derive neutral gas composition.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2016

THE SUBARCSECOND MID-INFRARED VIEW OF LOCAL ACTIVE GALACTIC NUCLEI. III. POLAR DUST EMISSION

Recent mid-infrared (MIR) interferometric observations have shown that in a few active galactic nuclei (AGNs) the bulk of the infrared emission originates from the polar region above the putative torus, where only a little dust should be present. Here, we investigate whether such strong polar dust emission is common in AGNs. Out of 149 Seyferts in the MIR atlas of local AGNs, 21 show extended MIR emission on single-dish images. In 18 objects, the extended MIR emission aligns with the position angle (PA) of the system axis, established by [O iii], radio, polarization, and maser-based PA measurements. The relative amount of resolved MIR emission is at least 40% and scales with the [O iv] fluxes, implying a strong connection between the extended continuum and [O iv] emitters. These results together with the radio-quiet nature of the Seyferts support the scenario that the bulk of MIR emission is emitted by dust in the polar region and not by the torus, which would demand a new paradigm for the infrared emission structure in AGNs. The current low detection rate of polar dust in the AGNs of the MIR atlas is explained by the lack of sufficient high-quality MIR data and the requirements on the orientation, strength of narrow-line region, and distance of the AGNs. The James Webb Space Telescope will enable much deeper nuclear MIR studies with comparable angular resolution, allowing us to resolve the polar emission and surroundings in most of the nearby AGNs.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2016

GAMMA-RAY BURST REVERSE SHOCK EMISSION IN EARLY RADIO AFTERGLOWS

Reverse shock (RS) emission from gamma-ray bursts is an important tool in investigating the nature of the ejecta from the central engine. If the magnetization of the ejecta is not high enough to suppress the RS, a strong RS emission component, usually peaking in the optical/IR band early on, would provide an important contribution to early afterglow light curve. In the radio band, synchrotron self-absorption may suppress early RS emission and also delay the RS peak time. In this paper, we calculate the self-absorbed RS emission in the radio band under different dynamical conditions. In particular, we stress that the RS radio emission is subject to self-absorption in both RSs and forward shocks (FSs). We calculate the ratio between the RS to FS flux at the RS peak time for different frequencies, which is a measure of the detectability of the RS emission component. We then constrain the range of physical parameters for a detectable RS, in particular the role of magnetization. We notice that unlike optical RS emission which is enhanced by moderate magnetization, moderately magnetized ejecta do not necessarily produce a brighter radio RS due to the self-absorption effect. For typical parameters, the RS emission component would not be detectable below 1 GHz unless the medium density is very low (e.g., n < 10{sup −3} cm{sup −3} for the interstellar medium and A {sub *} < 5 × 10{sup −4} for wind). These predictions can be tested using the afterglow observations from current and upcoming radio facilities such as the Karl G. Jansky Very Large Array, the Low-Frequency Array, the Five Hundred Meter Aperture Spherical Telescope, and the Square Kilometer Array.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2016

HARD X-RAY EMISSIONS FROM CASSIOPEIA A OBSERVED BY INTEGRAL

Cassiopeia A (Cas A), as the nearby young remnant of a core-collapse supernova, is the best candidate for astrophysical studies in supernova explosion and its environment. We studied the hard X-ray emission from Cas A using the 10 year data of INTEGRAL observations, and first detected non-thermal continuum emission from the source up to 220 keV. The {sup 44}Ti line emission at 68 and 78 keV is confirmed by our observations with a mean flux of ∼(2.2 ± 0.4) × 10{sup 5} ph cm{sup 2} s{sup 1}, corresponding to a {sup 44}Ti yield in Cas A of (1.3 ± 0.4) × 10{sup 4} M {sub ⊙}. The continuum emission from 3 to 500 keV can be fit with a thermal bremsstrahlung of kT ∼ 0.79 ± 0.08 keV plus a power-law model of Γ ∼ 3.13 ± 0.03. The non-thermal emission from Cas A is well fit by a power-law model without a cutoff up to 220 keV. This radiation characteristic is inconsistent with diffusive shock acceleration models with a remnant shock velocity of only 5000 km s{sup 1}. The central compact object in Cas A cannot significantly contribute to the emission above 80 keV. Some possible physical origins of the non-thermal emission above 80 keV from the remnant shock are discussed. We deduce that the asymmetrical supernova explosion scenario of Cas A is a promising scenario for the production of high-energy synchrotron radiation photons, where a portion of the ejecta with a velocity of ∼0.1 c and opening angle of ∼10° can account for the 100 keV emission, as is consistent with the “jet” observed in Cas A.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2017

A Catalog of GALEX Ultraviolet Emission from Asymptotic Giant Branch Stars

We have performed a comprehensive study of the UV emission detected from asymptotic giant branch (AGB) stars by the Galaxy Evolution Explorer (GALEX). Of the 468 AGB stars in our sample, 316 were observed by GALEX. In the near-UV (NUV) bandpass (λ{sub eff}∼2310 A-ring ), 179 AGB stars were detected and 137 were not detected. Only 38 AGB stars were detected in the far-UV (FUV) bandpass (λ{sub eff}∼1528 A-ring ). We find that NUV emission is correlated with optical to near-infrared emission, leading to higher detection fractions among the brightest, and hence closest, AGB stars. Comparing the AGB time-variable visible phased light curves to corresponding GALEX NUV phased light curves, we find evidence that for some AGB stars the NUV emission varies in phase with the visible light curves. We also find evidence that the NUV emission and possibly the FUV emission are anticorrelated with the circumstellar envelope density. These results suggest that the origin of the GALEX-detected UV emission is an inherent characteristic of the AGB stars that can most likely be traced to a combination of photospheric and chromospheric emission. In most cases, UV detections of AGB stars are not likely to be indicative of the presence of binary companions.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2017

Evidence of an Internal Dissipation Origin for the High-energy Prompt Emission of GRB 170214A

The origin of the prompt high-energy (>100 MeV) emission of gamma-ray bursts (GRBs), detected by the Large Area Telescope (LAT) on board the Fermi Gamma-ray Space Telescope, for which both an external shock origin and internal dissipation origin have been suggested, is still under debate. In the internal dissipation scenario, the high-energy emission is expected to exhibit significant temporal variability, tracking the keV/MeV fast variable behavior. Here, we report a detailed analysis of the Fermi data of GRB 170214A, which is sufficiently bright in high energies to enable a quantitative analysis of the correlation between high-energy emission and keV/MeV emission with high statistics. Our result shows a clear temporal correlation between high-energy and keV/MeV emission in the whole prompt emission phase as well as in two decomposed short time intervals. Such a correlation is also found in some other bright LAT GRBs, e.g., GRB 080916C, 090902B, and 090926A. For these GRBs as well as GRB 090510, we also find rapid temporal variability in the high-energy emission. We thus conclude that the prompt high-energy emission in these bright LAT GRBs should be due to an internal origin.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2016

EVIDENCE FOR NON-STELLAR REST-FRAME NEAR-IR EMISSION ASSOCIATED WITH INCREASED STAR FORMATION IN GALAXIES AT z ∼ 1

We explore the presence of non-stellar rest-frame near-IR (2–5 μm) emission in galaxies at z ∼ 1. Previous studies identified this excess in relatively small samples and suggested that such non-stellar emission, which could be linked to the 3.3 μm polycyclic aromatic hydrocarbons feature or hot dust emission, is associated with an increased star formation rate (SFR). In this Letter, we confirm and quantify the presence of an IR excess in a significant fraction of galaxies in the 3D-HST GOODS catalogs. By constructing a matched sample of galaxies with and without strong non-stellar near-IR emission, we find that galaxies with such emission are predominantly star-forming galaxies. Moreover, star-forming galaxies with an excess show increased mid- and far-IR and Hα emission compared to other star-forming galaxies without. While galaxies with a near-IR excess show a larger fraction of individually detected X-ray active galactic nuclei (AGNs), an X-ray stacking analysis, together with the IR-colors and Hα profiles, shows that AGNs are unlikely to be the dominant source of excess in the majority of galaxies. Our results suggest that non-stellar near-IR emission is linked to increased SFRs and is ubiquitous among star-forming galaxies. As such, the near-IR emission might be a powerful tool to measure SFRs in the era of the James Webb Space Telescope.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2016

ALMA 0.1–0.2 arcsec resolution imaging of the NGC 1068 Nucleus: compact dense molecular gas emission at the putative AGN location

We present the results of our ALMA Cycle 2 high angular resolution (0.″1–0.″2) observations of the nuclear region of the nearby well-studied type-2 active galactic nucleus (AGN), NGC 1068, at HCN J = 3–2 and HCO{sup +} J = 3–2 emission lines. For the first time, due to a higher angular resolution than previous studies, we clearly detected dense molecular gas emission at the putative AGN location, identified as a ∼1.1 mm (∼266 GHz) continuum emission peak, by separating this emission from brighter emission located at 0.″5–2.″0 on the eastern and western sides of the AGN. The estimated intrinsic molecular emission size and dense molecular mass, which are thought to be associated with the putative dusty molecular torus around an AGN, were ∼10 pc and ∼several × 10{sup 5} M {sub ⊙}, respectively. HCN-to-HCO{sup +} J = 3–2 flux ratios substantially higher than unity were found throughout the nuclear region of NGC 1068. The continuum emission displayed an elongated morphology along the direction of the radio jet located at the northern side of the AGN, as well as a weak spatially-resolved component at ∼2.″0 on the southwestern side of the AGN. The latter component most likely originated from star formation, with the estimated luminosity more than one order of magnitude lower than the luminosity of the central AGN. No vibrationally excited ( v {sub 2} = 1f) J = 3–2 emission lines were detected for HCN and HCO{sup +} across the field of view.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

Improved ELMv1-ECA simulations of zero-curtain periods and cold-season CH 4 and CO 2 emissions at Alaskan Arctic tundra sites

Field measurements have shown that cold-season methane (CH 4 ) and carbon dioxide (CO 2 ) emissions contribute a substantial portion to the annual net carbon emissions in permafrost regions. However, most earth system land models do not accurately reproduce cold-season CH 4 and CO 2 emissions, especially over the shoulder (i.e., thawing and freezing) seasons. Here we use the Energy Exascale Earth System Model (E3SM) land model version 1 (ELMv1-ECA) to tackle this challenge and fill the knowledge gap of how cold-season CH 4 and CO 2 emissions contribute to the annual totals at Alaska Arctic tundra sites. Specifically, we improved the ELMv1-ECA soil water phase-change scheme, environmental controls on microbial activity, and the methane module. Results demonstrate that both soil temperature and the duration of zero-curtain periods (i.e., the fall period when soil temperatures linger around 0°C) simulated by the updated ELMv1-ECA were greatly improved; e.g., the mean absolute error (MAE) in zero-curtain durations at 12 cm depth was reduced by 62 % on average. Furthermore, the MAEs of simulated cold-season carbon emissions at three tundra sites were improved by 72 % and 70 % on average for CH 4 and CO 2 , respectively. Overall, CH 4 emitted during the early cold season (September and October), which often includes most of the zero-curtain period in Arctic tundra, accounted for more than 50 % of the total emissions throughout the entire cold season (September to May) in the model, compared with around 49.4 % (43 %–58 %) in observations. From 1950 to 2017, both CO 2 emissions during the zero-curtain period and during the entire cold season showed increasing trends, for example, of 0.17 and 0.36 gC m -2 yr -1 at Atqasuk. This study highlights the importance of zero-curtain periods in facilitating cold-season CH 4 and CO 2 emissions from tundra ecosystems.

58 GEOSCIENCES↗

NASA NTRS2018

Top-Down NOx Emissions of European Cities Based on the Downwind Plume of Modelled and Space-Borne Tropospheric NO2 Columns

Top-down estimates of surface NOX emissions were derived for 23 European cities based on the downwind plume decay of tropospheric nitrogen dioxide (NO2) columns from the LOTOS-EUROS (Long Term Ozone Simulation-European Ozone Simulation) chemistry transport model (CTM) and from Ozone Monitoring Instrument (OMI) satellite retrievals, averaged for the summertime period (April-September) during 2013. Here we show that the top-down NOX emissions derived from LOTOS-EUROS for European urban areas agree well with the bottom-up NOX emissions from the MACC-III inventory data (R(exp 2) = 0.88) driving the CTM demonstrating the potential of this method. OMI top-down NOX emissions over the 23 European cities are generally lower compared with the MACC-III emissions and their correlation is slightly lower (R(exp 2) = 0.79). The uncertainty on the derived NO2 lifetimes and NOX emissions are on average ~55% for OMI and ~63% for LOTOS-EUROS data. The downwind NO2 plume method applied on both LOTOS-EUROS and OMI tropospheric NO2 columns allows to estimate NOX emissions from urban areas, demonstrating that this is a useful method for real-time updates of urban NOX emissions with reasonable accuracy.

NOx emissions↗

NASA NTRS2020

Inconsistencies in Sulphur Dioxide Emissions from the Canadian Oil Sands and Potential Implications

Satellite-derived and reported sulfur dioxide (SO2) emissions from the Canadian oil sands are shown to have been consistent up to 2013. Post-2013, these sources of emissions data diverged, with reported emissions dropping by a factor of two, while satellite-derived emissions for the region remained relatively constant, with the discrepancy (satellite-derived emissions minus reported emissions) peaking at 50 kt(SO2) yr−1 around 2016. The 2013–2014 period corresponds to when new flue-gas desulfurization units came on-line. Previous work has established a high level of consistency between at-stack SO2 emissions observations and satellite estimates, and surface monitoring network SO2 concentrations over the same multi-year period show similar trends as the satellite data, with a slight increase in concentrations post-2013. No clear explanation for this discrepancy currently exists. The implications of the discrepancy towards estimated total sulfur deposition to downwind ecosystems were estimated relative to 2013 emissions levels, with the satellite-derived values leaving the area of regional critical load exceedances of aquatic ecosystems largely unchanged from 2013 values, 335 000 km2, and reported values potentially decreasing this area to 185,000 km2.

Sulphur dioxide (SO2) emissions↗

NASA NTRS2022

Changes in Anthropogenic Precursor Emissions Drive Shifts in the Ozone Seasonal Cycle Throughout the Northern Midlatitude Troposphere

Simulations by six Coupled Model Intercomparison Project Phase 6 (CMIP6) Earth system models indicate that the seasonal cycle of baseline tropospheric ozone at northern midlatitudes has been shifting since the mid-20th century. Beginning in ∼ 1940, the magnitude of the seasonal cycle increased by ∼10 ppb (measured from seasonal minimum to maximum), and the seasonal maximum shifted to later in the year by about 3 weeks. This shift maximized in the mid-1980s, followed by a reversal – the seasonal cycle decreased in amplitude and the maximum shifted back to earlier in the year. Similar changes are seen in measurements collected from the 1970s to the present. The timing of the seasonal cycle changes is generally concurrent with the rise and fall of anthropogenic emissions that followed industrialization and the subsequent implementation of air quality emission controls. A quantitative comparison of the temporal changes in the ozone seasonal cycle at sites in both Europe and North America with the temporal changes in ozone precursor emissions across the northern midlatitudes found a high degree of similarity between these two temporal patterns. We hypothesize that changing precursor emissions are responsible for the shift in the ozone seasonal cycle; this is supported by the absence of such seasonal shifts in southern midlatitudes where anthropogenic emissions are much smaller. We also suggest a mechanism by which changing emissions drive the changing seasonal cycle: increasing emissions of NOx allow summertime photochemical production of ozone to become more important than ozone transported from the stratosphere, and increasing volatile organic compounds (VOCs) lead to progressively greater photochemical ozone production in the summer months, thereby increasing the amplitude of the seasonal ozone cycle. Decreasing emissions of both precursor classes then reverse these changes. The quantitative parameter values that characterize the seasonal shifts provide useful benchmarks for evaluating model simulations, both against observations and between models.

Ozone↗