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At least 19 records

Influence of Dynamic Ozone Dry Deposition on Ozone Pollution

Identifying the contributions of chemistry and transport to observed ozone pollution using regional‐to‐global models relies on accurate representation of ozone dry deposition. We use a recently developed configuration of the NOAA GFDL chemistry‐climate model – in which the atmosphere and land are coupled through dry deposition—to investigate the influence of ozone dry deposition on ozone pollution over northern midlatitudes. In our model, deposition pathways are tied to dynamic terrestrial processes, such as photosynthesis and water cycling through the canopy and soil. Small increases in winter deposition due to more process‐based representation of snow and deposition to surfaces reduce hemispheric‐scale ozone throughout the lower troposphere by 5–12 ppb, improving agreement with observations relative to a simulation with the standard configuration for ozone dry deposition. Declining snow cover by the end of the 21st‐century tempers the previously identified influence of rising methane on winter ozone. Dynamic dry deposition changes summer surface ozone by −4 to +7 ppb. While previous studies emphasize the importance of uptake by plant stomata, new diagnostic tracking of depositional pathways reveals a widespread impact of nonstomatal deposition on ozone pollution. Daily variability in both stomatal and nonstomatal deposition contribute to daily variability in ozone pollution. Twenty‐first century changes in summer deposition result from a balance among changes in individual pathways, reflecting differing responses to both high carbon dioxide (through plant physiology versus biomass accumulation) and water availability. Our findings highlight a need for constraints on the processes driving ozone dry deposition to test representation in regional‐to‐global models.

dry deposition↗

Tropospheric Ozone Pollution Transport Traced from the TOMS (Total Ozone Mapping Spectrometer) Instrument During the Nashville-1999 Campaign

Over the past several years, we have developed two new tropospheric ozone retrievals from the TOMS (Total Ozone Mapping Spectrometer) satellite instrument that are of sufficient resolution to follow pollution episodes. The modified-residual technique [Hudson and Thompson, 1998; Thompson and Hudson, 1999] uses v. 7 TOMS total ozone and is applicable to tropical regimes in which the wave-one pattern in total ozone is observed. The TOMS-direct method [("TDOT" = TOMS Direct Ozone in the Troposphere; Frolov et al., 2000] represents a new algorithm that uses TOMS radiances directly (i.e., not previously processed for TOMS ozone) to extract tropospheric ozone in regions of constant stratospheric ozone and tropospheric ozone displaying high mixing ratios and variability characteristic of pollution. These events tend to occur in certain meteorological regimes. For example, mid-latitude pollution usually occurs on the backside of subtropical fronts, as low pv, usually moist air intrudes to the extra-tropics. July 1999 was a month characterized by robust pollution in the eastern US, with high ozone, as detected by TOMS, originating over south central states and moving up the Atlantic seaboard. This corresponds to 50-80 DU in tropospheric ozone column depth. In most cases, further transport occurred to the North Atlantic, with ozone plumes traveling to western Europe in 4-5 days. Examples of high ozone and transit across boundaries within the US, as well as US->Europe, give a regional context for model results and field measurements taken in the SE US during the Nashville-1999 campaign period. Validation of the TDOT maps is made with ozonesondes taken during that time. TDOT maps also show ozone pollution from Asia traveling to the western US in July 1999.

Thompson, Anne M.↗

Tropospheric Ozone Pollution from Space: New Views from the TOMS (Total Ozone Mapping Spectrometer) Instrument

New products from the TOMS (Total Ozone Mapping Spectrometer) >satellite instrument can resolve pollution events in tropical and mid-latitudes, Over the past several years, we have developed tropospheric ozone data sets by two methods. The modified-residual technique [Hudson and Thompson, 1998; Thompson and Hudson, 1999] uses v. 7 TOMS total ozone and is applicable to tropical regimes in which the wave-one pattern in total ozone is observed. The TOMSdirect method [Hudson et at., 2000] represents a new algorithm that uses TOMS radiances to extract tropospheric ozone in regions of constant stratospheric ozone and tropospheric ozone displaying high mixing ratios and variability characteristic of pollution, Absorbing aerosols (dust and smoke; Herman et at., 1997 Hsu et al., 1999), a standard TOMS product, provide transport and/or source marker information to interpret tropospheric ozone. For the Nimbus 7/TOMS observing period (1979-1992), modified-residual TTO (tropical tropospheric ozone) appears as two maps/month at I-degree latitude 2-degree longitude resolution at a homepage and digital data are available (20S to 20N) by ftp at http://metosrv2. umd.edu/~tropo/ 14y_data.d. Preliminary modified-residual TTO data from the operational Earth-Probe/TOMS (1996- present) are posted in near-real-time at the same website. Analyses with the new tropospheric ozone and aerosol data are illustrated by the following (I)Signals in tropical tropospheric ozone column and smoke amount during ENSO (El Nino-Southern Oscillation) events, e.g. 1982-1983 and the intense ENSO induced biomass fires of 1997-1998 over the Indonesian region [Thompson et a[, 2000a, Thompson and Hudson, 1999]. (2) Trends in tropospheric ozone and smoke aerosols in various tropical regions (Atlantic, Pacific, Africa, Brazil). No significant trends were found for ozone from1980-1990 [Thompson and Hudson, 19991 although smoke aerosols increased during the period [Hsu et al.,1999]. (3) Temporal and spatial offsets ("paradoxes") in tropical tropospheric ozone and smoke aerosol in regions of greatest tropical biomass burning [Thompson et at., 1996;2000b]. (4) Trans-boundary pollution tracking. With an air parcel (trajectory) model, smoke aerosol and ozone and dust plumes can be tracked across oceans (e.g., Asia to North America; North America to Europe) and national boundaries, e.g. Indonesia to Singapore and Malaysia during the 1997 ENSO fires.

Thompson, Anne M.↗

Three-D Simulation of the Origin of the Pollutant Ozone Maxima in the Great African Plume: New Meteorology, New Chemistry for TRACE-A

Burning in South Central Africa is primarily responsible for the vast buildup of ozone in the mid-Atlantic noticeable in the Belem, Brazil, ozonesondes, and also visible in analyses using the Total Ozone Mapping Spectrometer (TOMS). We report on full-scale chemistry simulations for the SAFARI/TRACE-A field period of September-October, 1992. These observational programs provided a wealth of comparison data, including spectacular depictions of the vertical structure of ozone and particulate pollution over Africa, South America, and the Equatorial Atlantic [Browell JGR, 1996, submitted] above and below the NASA DC-8 airplane path. These depictions provide strict tests on the ability of a 3-d simulation and its controlling input parameters, most notably the biomass burning emissions strength. We use meteorology from MM5 used as a synoptic assimilation model and our own GRACES Global Regional Air Chemistry Event Simulator. This report will focus on the unique meteorology of the Equatorial Atmosphere around the Gulf of Guinea during the TRACE-A period, which we describe as "the opening of the gate," "the Great African Plume," and the "African Recirculatory System." We expect to assess whether the ozone observed is primarily "transported African smog," the standard view, or whether "re-$NO_[x)$-ification" of the Central Atlantic troposphere (reduction of nitric acid to active nitrogen oxides in clouds or aerosol) may be required for "extended intercontinental ozone production." A status report on a second nitrogen problem, "lower-tropospheric missing NO(y)," in which we find a serious imbalance in the $NO_ {x }$ and $NO_{y}$ budgets when compared with similar atmospheric tracers, will be given. An elaboration of the concepts set off by quotation marks in this abstract will be given in the talk.

Chatfeild, Robert↗

Lusaka, Zambia during SAFARI-2000: A Collection Point for Ozone Pollution

In August and September, throughout south central Africa, seasonal clearing of dry vegetation and other fire-related activities lead to intense smoke haze and ozone formation. The first ozone soundings in the heart of the southern African burning region were taken at Lusaka, Zambia (155 deg S, 28 deg E) in early September 2000. Over 90 ppbv ozone was recorded at the surface (1.3 km elevation) and column tropospheric ozone was greater than 50 DU during a stagnant period. These values are much higher than concurrent measurements over Nairobi (1 deg S, 38 deg E) and Irene (25 deg S, 28 deg E, near Pretoria). The heaviest ozone pollution layer (800-500 hPa) over Lusaka is due to recirculated trans-boundary ozone. Starting out over Zambia, Angola, and Namibia, ozone heads east to the Indian Ocean, before turning back over Mozambique and Zimbabwe, heading toward Lusaka. Thus, Lusaka is a collection point for pollution, consistent with a picture of absolutely stable layers recirculating in a gyre over southern Africa.

Thompson, Anne M.↗

Discoveries about Tropospheric Ozone Pollution from Satellite and Sounding

We have been producing near-real time tropospheric ozone satellite maps from the TOMS (Total Ozone Mapping Spectrometer) sensor since 1997. This is most readily done for the tropics, where the stratospheric and tropospheric ozone column amounts can be discriminated readily. Maps for 1996-2000 for the operational Earth-Probe instrument reside at: chttp://www.atmos.umd.edu/-trope>. Pollution in the tropics is influenced by biomass burning and by transport patterns that favor recirculation and in other cases reflect climate variability like the El-Nino-Southern Oscillation [Thompson et al., 2001]. Time permitting, examples of mid-latitude, intercontinental transport of ozone pollution sensed by TOMS will be shown. The satellite view of chemical-dynamical interactions in tropospheric ozone is not adequate to capture vertical variability. Thus, in 1998, NASA's Goddard Space Flight Center and a team of international sponsors established the SHADOZ (Southern Hemisphere ADditional OZonesondes) project to address the gap in tropical ozone soundings. SHADOZ augments launches and provides a public archive of ozonesonde data from twelve tropical stations at http://croc.gsfc.nasa.gov/shadoz. Further insights into the role of chemical and dynamical influences have emerged from the first 4-5 years of SHADOZ data (less than 2000 ozone profiles): (a) highly variable tropospheric ozone; (b) a zonal wave-one pattern in tropospheric column ozone; (c) convective variability affects tropospheric ozone over the Indian and Pacific Ocean; (d) a "tropical Atlantic Paradox" appears in December-January-February.

Thompson, Anne M.↗

Discoveries about Tropospheric Ozone Pollution from Satellite and Soundings

We have been producing near-red time tropospheric ozone satellite maps from the TOMS (Total Ozone Mapping Spectrometer) sensor since 1997. Maps for 1996-2000 for the operational Earth-Probe instrument are at: . Pollution in the tropics is influenced by biomass burning and by transport patterns that favor recirculation and in other cases reflect climate variability like the El-Nino-Southern Oscillation [Thompson et al., 2001]. The satellite view of chemical-dynamical interactions in tropospheric ozone is not adequate to capture vertical gradients in pollution. Thus, in 1998, NASA's Goddard Space Flight Center and a team of international sponsors established the SHADOZ (Southern Hemisphere ADditional OZonesondes) project to address the gap in tropical ozone soundings. SHADOZ augments launches and provides a public archive of ozonesonde data from twelve tropical stations at http://croc.gsfc.nasa.gov/shadoz. Further insights into the role of chemical and dynamical influences have emerged from the first 4-5 years of SHADOZ data (more than 2000 ozone profiles). Highly variable tropospheric ozone and a zonal wave-one pattern in tropospheric ozone suggest that dynamics is as important as pollution in determining tropical ozone distributions.

Thompson, Anne M.↗

Ozone Pollution, Transport and Variability: Examples from Satellite and In-Situ Observations

Regional and intercontinental transport of ozone has been observed from satellite, aircraft and sounding data. Over the past several years, we have developed new tropospheric ozone retrieval techniques from the TOMS (Total Ozone Mapping Spectrometer) satellite instrument that are of sufficient resolution to follow pollution episodes. The modified-residual technique uses Level 2 total ozone and was used to follow the 1997 fires in the wake of the El-Nino-related fires in southeast Asia and the Indonesian maritime continent. The TOMS-direct method ('TDOT' = TOMS Direct Ozone in the Troposphere) is a newer algorithm that uses TOMS radiances directly to extract tropospheric ozone. Ozonesonde data that have been taken in campaigns (e.g. TRACE-P) and more consistently in the SHADOZ (Southern Hemisphere Additional Ozonesondes) project, reveal layers of pollution traceable with trajectories. Examples will be shown of long-range transport and recirculation over Africa during SAFARI-2000.

Thompson, Anne↗

Urban and Rural Ozone Pollution Over Lusaka (Zambia, 15.5S, 25E) During SAFARI-2000 (September 2000)

In early September, throughout south central Africa, seasonal clearing of dry vegetation and the production of charcoal for cooking leads to intense smoke haze and ozone formation. Ozone soundings made over Lusaka during a six-day period in early September 2000 recorded layers of high ozone (greater than 125 ppbv at 5 km) during two stagnant periods, interspersed by a frontal passage that reduced boundary layer ozone by 30 percent. Smoke aerosol column variations aloft and total ozone were monitored by a sun photometer. During the 6-day measurement period, surface ozone concentrations ranged from 50-95 ppbv and integrated tropospheric ozone from the soundings was 39- 54 Dobson Units (note 1.3 km elevation at the launch site). High ozone concentrations above the mixed and inversion layers were advected from rural burning regions in western Zambia where SAFARI aircraft and ground-based instruments observed intense biomass fires and elevated aerosol and trace gas amounts. TOMS tropospheric ozone and smoke aerosols products show the distribution of biomass burning and associated pollution throughout southern Africa in September 2000. Animations of satellite images and trajectories confirm pollutant recirculation over south central African fires, exit of ozone from Mozambique and Tanzania to the Indian Ocean and the characteristic buildup of tropospheric ozone over the Atlantic from western African outflow.

Thompson, Anne M.↗

The Dynamical Role of the Chesapeake Bay on the Local Ozone Pollution Using Mesoscale Modeling—A Case Study

This study investigated the dynamic influence of the Chesapeake Bay (CB) on local ozone (O3) concentration and distribution using a weather forecasting model. The Weather Research and Forecasting model coupled with Chemistry (WRF–Chem) was employed to simulate O3 production and transportation near the CB. Baseline (water) as well as sensitivity (nowater) model experiments of bay circulation were carried out with and without bay water by changing the water surface from water to land (loam). First, the model performance simulating O3 was evaluated using the baseline experiment results and AirNow surface wind and O3 observations. The results showed that the model overestimates surface O3 by up to 20–30%. Further, the comparisons of the baseline and sensitivity experiments revealed higher O3 mixing ratios, primarily due to the resulting bay breeze circulation. These increases, after considering model overestimation, represent a mean bay dynamics circulation-induced contribution of up to 10% at night and 5% during the day. Furthermore, the boundary layer over northern CB, where it is at its narrowest width, was higher (by 1.2 km on average) during daytime due to higher surface temperatures observed. The boundary layer depth difference between the northern, central, and southern regions of the bay leads to a differential in the role of bay circulation dynamics in the observed O3 increase. The relatively wider swath of water surface over southern CB resulted in a lower boundary layer depth and stronger breeze circulation and this circulation contributed to O3 concentrations. Moreover, since the case selected has a minimal bay breeze circulation, the associated surface ozone enhancements represent what is expected at least at a minimum.

Chesapeak Bay↗

Impacts of Climate Change on Surface Ozone and Intercontinental Ozone Pollution: A Multi-Model Study

The impact of climate change between 2000 and 2095 SRES A2 climates on surface ozone (O)3 and on O3 source-receptor (S-R) relationships is quantified using three coupled climate-chemistry models (CCMs). The CCMs exhibit considerable variability in the spatial extent and location of surface O3 increases that occur within parts of high NOx emission source regions (up to 6 ppbv in the annual average and up to 14 ppbv in the season of maximum O3). In these source regions, all three CCMs show a positive relationship between surface O3 change and temperature change. Sensitivity simulations show that a combination of three individual chemical processes-(i) enhanced PAN decomposition, (ii) higher water vapor concentrations, and (iii) enhanced isoprene emission-largely reproduces the global spatial pattern of annual-mean surface O3 response due to climate change (R2 = 0.52). Changes in climate are found to exert a stronger control on the annual-mean surface O3 response through changes in climate-sensitive O3 chemistry than through changes in transport as evaluated from idealized CO-like tracer concentrations. All three CCMs exhibit a similar spatial pattern of annual-mean surface O3 change to 20% regional O3 precursor emission reductions under future climate compared to the same emission reductions applied under present-day climate. The surface O3 response to emission reductions is larger over the source region and smaller downwind in the future than under present-day conditions. All three CCMs show areas within Europe where regional emission reductions larger than 20% are required to compensate climate change impacts on annual-mean surface O3.

Troposphere: constituent transport and chemistry↗

Asian Outflow and Trans-Pacific Transport of Carbon Monoxide and Ozone Pollution: An Integrated Satellite, Aircraft, and Model Perspective

Satellite observations of carbon monoxide (CO) from the Measurements of Pollution in the Troposphere (MOPITT) instrument are combined with measurements from the Transport and Chemical Evolution Over the Pacific (TRACE-P) aircraft mission over the northwest Pacific and with a global three-dimensional chemical transport model (GEOS-CHEM) to quantify Asian pollution outflow and its trans-Pacific transport during spring 2001. Global CO column distributions in MOPITT and GEOS-CHEM are highly correlated (R(exp 2) = 0.87), with no significant model bias. The largest regional bias is over Southeast Asia, where the model is 18% too high. A 60% decrease of regional biomass burning emissions in the model (to 39 Tg/yr) would correct the discrepancy; this result is consistent with TRACE-P observations. MOPITT and TRACE-P also give consistent constraints on the Chinese source of CO from fuel combustion (181 Tg CO/yr). Four major events of trans-Pacific transport of Asian pollution in spring 2001 were seen by MOPITT, in situ platforms, and GEOS-CHEM. One of them was sampled by TRACE-P (26-27 February) as a succession of pollution layers over the northeast Pacific. These layers all originated from one single event of Asian outflow that split into northern and southern plumes over the central Pacific. The northern plume (sampled at 6-8 km off California) had no ozone enhancement. The southern subsiding plume (sampled at 2-4 km west of Hawaii) contained a 8 - 17 ppbv ozone enhancement, driven by decomposition of peroxyacetylnitrate (PAN) to nitrogen oxides (NOx). This result suggests that PAN decomposition in trans-Pacific pollution plumes subsiding over the United States could lead to significant enhancements of surface ozone.

Heald, Colette L.↗

Evaluating a Priori Ozone Profile Information Used in TEMPO (Tropospheric Emissions: Monitoring of Pollution) Tropospheric Ozone Retrievals

A primary objective for TOLNet is the evaluation and validation of space-based tropospheric O3 retrievals from future systems such as the Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite. This study is designed to evaluate the tropopause-based O3 climatology (TB-Clim) dataset which will be used as the a priori profile information in TEMPO O3 retrievals. This study also evaluates model simulated O3 profiles, which could potentially serve as a priori O3 profile information in TEMPO retrievals, from near-real-time (NRT) data assimilation model products (NASA Global Modeling and Assimilation Office (GMAO) Goddard Earth Observing System (GEOS-5) Forward Processing (FP) and Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA2)) and full chemical transport model (CTM), GEOS-Chem, simulations. The TB-Clim dataset and model products are evaluated with surface (0-2 km) and tropospheric (0-10 km) TOLNet observations to demonstrate the accuracy of the suggested a priori dataset and information which could potentially be used in TEMPO O3 algorithms. This study also presents the impact of individual a priori profile sources on the accuracy of theoretical TEMPO O3 retrievals in the troposphere and at the surface. Preliminary results indicate that while the TB-Clim climatological dataset can replicate seasonally-averaged tropospheric O3 profiles observed by TOLNet, model-simulated profiles from a full CTM (GEOS-Chem is used as a proxy for CTM O3 predictions) resulted in more accurate tropospheric and surface-level O3 retrievals from TEMPO when compared to hourly (diurnal cycle evaluation) and daily-averaged (daily variability evaluation) TOLNet observations. Furthermore, it was determined that when large daily-averaged surface O3 mixing ratios are observed (65 ppb), which are important for air quality purposes, TEMPO retrieval values at the surface display higher correlations and less bias when applying CTM a priori profile information compared to all other data products. The primary reason for this is that CTM predictions better capture the spatio-temporal variability of the vertical profiles of observed tropospheric O3 compared to the TB-Clim dataset and other NRT data assimilation models evaluated during this study.

Pollution↗

Systems theoretic model of stratospheric pollution on ozone

Discrete state space analysis is applied to the development of a model for predicting the reduction in the amount of stratospheric ozone due to stratospheric pollution. The modeling approach is to segment the stratosphere into a number of altitudinal bands and to associate state variables with the state of ozone reduction in each band due to NO(x) injections. The ozone reductions in each band are then combined into an estimate of total global ozone reduction. The model proposed predicts changes in stratospheric ozone based on altitude of pollutant injection and volume of pollutant injected at that altitude. The present approach is not a detailed analysis of stratospheric constituents and their interactions, but rather an analysis procedure for modeling the results of other researchers in the field.

Wilkins, R. D.↗

The Influence of European Pollution on Ozone in the Near East and Northern Africa

We present a modeling study of the long-range transport of pollution from Europe, showing that European emissions regularly elevate surface ozone by as much as 20 ppbv in summer in northern Africa and the Near East. European emissions cause 50-150 additional violations per year (i.e. above those that would occur without European pollution) of the European health standard for ozone (8-h average greater than 120 micrograms per cubic meters or approximately 60 ppbv) in northern Africa and the Near East. We estimate that European ozone pollution is responsible for 50 000 premature mortalities globally each year, of which the majority occurs outside of Europe itself, including 37% (19 000) in northern Africa and the Near East. Much of the pollution from Europe is exported southward at low altitudes in summer to the Mediterranean Sea, northern Africa and the Near East, regions with favorable photochemical environments for ozone production. Our results suggest that assessments of the human health benefits of reducing ozone precursor emissions in Europe should include effects outside of Europe, and that comprehensive planning to improve air quality in northern Africa and the Near East likely needs to address European emissions.

Duncan, B. N.↗

Distribution of tropospheric ozone in the tropics from satellite and ozonesonde measurements

Measurements from two independent satellite data sets have been used to derive the climatology of the integrated amount of ozone in the troposphere. These data have led to the finding that large amounts of ozone pollution are generated by anthropogenic activity originating from both the industrialized regions of the Northern Hemisphere and from the southern tropical regions of Africa. To verify the existence of this ozone anomaly over this region of the world, an ozonesonde capability has been established at Ascension Island, located downwind of the primary source region of this ozone pollution, which likely results from the photochemical oxidation of emissions emanating from the widespread burning of savanna. These first ozonesonde profiles suggest that much of the ozone generated over Africa during the 'burning season' (primarily July-October) reaches Ascension Island. These high levels of ozone in the lower troposphere become much lower by December. Elevated ozone concentrations in the middle troposphere are once again evident in February, which may be the result of biomass burning emissions being transported from western and northern Africa.

Fishman, J.↗

The use of satellite data to determine the distribution of ozone in the troposphere

Measurements from two independent satellite data sets have been used to derive the climatology of the integrated amount of ozone in the troposphere. These data have led to the finding that large amounts of ozone pollution are generated by anthropogenic activity originating from both the industrialized regions of the Northern Hemisphere and from the southern tropical regions of Africa. To verify the existence of this ozone anomaly at low latitudes, an ozonesonde capability has been established at Ascension Island (8 deg S, 15 deg W) since July 1990. According to the satellite analyses, Ascension Island is located downwind of the primary source region of this ozone pollution, which likely results from the photochemical oxidation of emissions emanating from the widespread burning of savannas and other biomass. These in situ measurements confirm the existence of large amounts of ozone in the lower atmosphere. A summary of these ozonesonde data to date will be presented. In addition, we will present some ozone profile measurements from SAGE II which can be used to provide upper tropospheric ozone measurements directly in the tropical troposphere. A preliminary comparison between the satellite observations and the ozonesonde profiles in the upper troposphere and lower stratosphere will also be presented.

Fishman, Jack↗

Science Accomplishments from a Decade of Aura OMI/MLS Tropospheric Ozone Measurements

Measurements of tropospheric ozone from combined Aura OMI and MLS instruments have yielded a large number of new and important science discoveries over the last decade. These discoveries have generated a much greater understanding of biomass burning, lightning NO, and stratosphere-troposphere exchange sources of tropospheric ozone, ENSO dynamics and photochemistry, intra-seasonal variability-Madden-Julian Oscillation including convective transport, radiative forcing, measuring ozone pollution from space, improvements to ozone retrieval algorithms, and evaluation of chemical-transport and chemistry-climate models. The OMI-MLS measurements have been instrumental in giving us better understanding of the dynamics and chemistry involving tropospheric ozone and the many drivers affecting the troposphere in general. This discussion will provide an overview focusing on our main science results.

ENSO↗