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NASA NTRS2020

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↗
NASA NTRS2020

Observed Modulation of the Tropical Radiation Budget by Deep Convective Organization and Lower-Tropospheric Stability

This study analyses the observed monthly deseasonalized and detrended variability of the tropical radiation budget, and suggests that variations of the lower-tropospheric stability and of the spatial organization of deep convection both strongly contribute to this variability. Satellite observations show that on average over the tropical belt, when deep convection is more aggregated, the free troposphere is drier, the deep-convective cloud coverage is less extensive, and the emission of heat to space is increased; an enhanced aggregation of deep convection is thus associated with a radiative cooling of the tropics. An increase of the tropical-mean lower-tropospheric stability is also coincident with a radiative cooling of the tropics, primarily because it is associated with more marine low clouds and an enhanced reflection of solar radiation, although the free-tropospheric drying also contributes to the cooling. The contributions of convective aggregation and lower-tropospheric stability to the modulation of the radiation budget are complementary, largely independent of each other, and equally strong. Together, they account for more than sixty percent of the variance of the tropical radiation budget. Satellite observations are thus consistent with the suggestion from modeling studies that the spatial organization of deep convection substantially influences the radiative balance of the Earth. This emphasizes the importance of understanding the factors that control convective organization and lower-tropospheric stability variations, and the need to monitor their changes as the climate warms.

convective aggregation↗
NASA NTRS2023

Characterization of Errors in Satellite-Based HCHO/NO 2 Tropospheric Column Ratios With Respect to Chemistry, Column-to-PBL Translation, Spatial Representation, and Retrieval Uncertainties

The availability of formaldehyde (HCHO) (a proxy for volatile organic compound reactivity) and nitrogen dioxide (NO 2 ) (a proxy for nitrogen oxides) tropospheric columns from ultraviolet–visible (UV–Vis) satellites has motivated many to use their ratios to gain some insights into the near-surface ozone sensitivity. Strong emphasis has been placed on the challenges that come with transforming what is being observed in the tropospheric column to what is actually in the planetary boundary layer (PBL) and near the surface; however, little attention has been paid to other sources of error such as chemistry, spatial representation, and retrieval uncertainties. Here we leverage a wide spectrum of tools and data to quantify those errors carefully. Concerning the chemistry error, a well-characterized box model constrained by more than 500 h of aircraft data from NASA's air quality campaigns is used to simulate the ratio of the chemical loss of HO 2 + RO 2 (LRO x ) to the chemical loss of NO x (LNO x ). Subsequently, we challenge the predictive power of HCHO/NO 2 ratios (FNRs), which are commonly applied in current research, in detecting the underlying ozone regimes by comparing them to LRO x /LNO x . FNRs show a strongly linear (R 2 =0.94) relationship with LRO x /LNO x , but only on the logarithmic scale. Following the baseline (i.e., ln(LRO x /LNO x ) = −1.0 ± 0.2) with the model and mechanism (CB06, r2) used for segregating NO x -sensitive from VOC-sensitive regimes, we observe a broad range of FNR thresholds ranging from 1 to 4. The transitioning ratios strictly follow a Gaussian distribution with a mean and standard deviation of 1.8 and 0.4, respectively. This implies that the FNR has an inherent 20 % standard error (1σ) resulting from not accurately describing the RO x –HO x cycle. We calculate high ozone production rates (PO 3 ) dominated by large HCHO × NO 2 concentration levels, a new proxy for the abundance of ozone precursors. The relationship between PO 3 and HCHO × NO 2 becomes more pronounced when moving towards NO x -sensitive regions due to nonlinear chemistry; our results indicate that there is fruitful information in the HCHO × NO 2 metric that has not been utilized in ozone studies. The vast amount of vertical information on HCHO and NO 2 concentrations from the air quality campaigns enables us to parameterize the vertical shapes of FNRs using a second-order rational function permitting an analytical solution for an altitude adjustment factor to partition the tropospheric columns into the PBL region. We propose a mathematical solution to the spatial representation error based on modeling isotropic semivariograms. Based on summertime-averaged data, the Ozone Monitoring Instrument (OMI) loses 12 % of its spatial information at its native resolution with respect to a high-resolution sensor like the TROPOspheric Monitoring Instrument (TROPOMI) (> 5.5 × 3.5 km 2 ). A pixel with a grid size of 216 km 2 fails at capturing ∼ 65 % of the spatial information in FNRs at a 50 km length scale comparable to the size of a large urban center (e.g., Los Angeles). We ultimately leverage a large suite of in situ and ground-based remote sensing measurements to draw the error distributions of daily TROPOMI and OMI tropospheric NO 2 and HCHO columns. At a 68 % confidence interval (1σ), errors pertaining to daily TROPOMI observations, either HCHO or tropospheric NO 2 columns, should be above 1.2–1.5 × 10 16 molec. cm −2 to attain a 20 %–30 % standard error in the ratio. This level of error is almost non-achievable with the OMI given its large error in HCHO. The satellite column retrieval error is the largest contributor to the total error (40 %–90 %) in the FNRs. Due to a stronger signal in cities, the total relative error (< 50 %) tends to be mild, whereas areas with low vegetation and anthropogenic sources (e.g., the Rocky Mountains) are markedly uncertain (> 100 %). Our study suggests that continuing development in the retrieval algorithm and sensor design and calibration is essential to be able to advance the application of FNRs beyond a qualitative metric.

Amir H. Souri↗
NASA NTRS2014

Volcanic Contribution to Decadal Changes in Tropospheric Temperature

Despite continued growth in atmospheric levels of greenhouse gases, global mean surface and tropospheric temperatures have shown slower warming since 1998 than previously. Possible explanations for the slow-down include internal climate variability, external cooling influences and observational errors. Several recent modelling studies have examined the contribution of early twenty-first-century volcanic eruptions to the muted surface warming. Here we present a detailed analysis of the impact of recent volcanic forcing on tropospheric temperature, based on observations as well as climate model simulations. We identify statistically significant correlations between observations of stratospheric aerosol optical depth and satellite-based estimates of both tropospheric temperature and short-wave fluxes at the top of the atmosphere. We show that climate model simulations without the effects of early twenty-first-century volcanic eruptions overestimate the tropospheric warming observed since 1998. In two simulations with more realistic volcanic influences following the 1991 Pinatubo eruption, differences between simulated and observed tropospheric temperature trends over the period 1998 to 2012 are up to 15% smaller, with large uncertainties in the magnitude of the effect. To reduce these uncertainties, better observations of eruption-specific properties of volcanic aerosols are needed, as well as improved representation of these eruption-specific properties in climate model simulations.

Atmospheric temperature↗
NASA NTRS2014

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↗
NASA NTRS2015

Impact of Stratospheric Ozone Zonal Asymmetries on the Tropospheric Circulation

The depletion and recovery of Antarctic ozone plays a major role in changes of Southern Hemisphere (SH) tropospheric climate. Recent studies indicate that the lack of polar ozone asymmetries in chemistry climate models (CCM) leads to a weaker and warmer Antarctic vortex, and smaller trends in the tropospheric mid-latitude jet and the surface pressure. However, the tropospheric response to ozone asymmetries is not well understood. In this study we report on a series of integrations of the Goddard Earth Observing System Chemistry Climate Model (GEOS CCM) to further examine the effect of zonal asymmetries on the state of the stratosphere and troposphere. Integrations with the full, interactive stratospheric chemistry are compared against identical simulations using the same CCM except that (1) the monthly mean zonal mean stratospheric ozone from first simulation is prescribed and (2) ozone is relaxed to the monthly mean zonal mean ozone on a three day time scale. To analyze the tropospheric response to ozone asymmetries, we examine trends and quantify the differences in temperatures, zonal wind and surface pressure among the integrations.

Chemistry-Climate Modeling↗
NASA NTRS2016

Tropospheric Ozone Source Attribution in Southern California during Summer 2014 Based on Lidar Measurements and Model Simulations

In the past decades, significant efforts have been made to increase tropospheric ozone long-term monitoring. A large number of ground-based, airborne and space-borne instruments are currently providing valuable data to contribute to better understand tropospheric ozone budget and variability. Nonetheless, most of these instruments provide in-situ surface and column-integrated data, whereas vertically resolved measurements are still scarce. Besides ozonesondes and aircraft, lidar measurements have proven to be valuable tropospheric ozone profilers. Using the measurements from the tropospheric ozone differential absorption lidar (DIAL) located at the JPL Table Mountain Facility, California, and the GEOS-Chem and GEOS-5 model outputs, the impact of the North American monsoon on tropospheric ozone during summer 2014 is investigated. The influence of the Monsoon lightning-induced NOx will be evaluated against other sources (e.g. local anthropogenic emissions and the stratosphere) using also complementary data such as backward-trajectories analysis, coincident water vapor lidar measurements, and surface ozone in-situ measurements.

Lidar↗
NASA NTRS2016

Understanding the Laminar Distribution of Tropospheric Ozone from Ground-Based, Airborne, Spaceborne, and Modeling Perspectives

Laminar ozone structure is a ubiquitous feature of tropospheric-ozone distributions resulting from dynamic and chemical atmospheric processes. Understanding the characteristics of these ozone laminae and the mechanisms responsible for producing them is important to outline the transport pathways of trace gases and to quantify the impact of different sources on tropospheric background ozone. In this study, we present a new method to detect ozone laminae to understand their climatological characteristics of occurrence frequency in terms of thickness and altitude. We employ both ground-based and airborne ozone lidar measurements and other synergistic observations and modeling to investigate the sources and mechanisms such as biomass burning transport, stratospheric intrusion, lightning-generated NOx, and nocturnal low-level jets that are responsible for depleted or enhanced tropospheric ozone layers. Spaceborne (e.g., OMI (Ozone Monitoring Instrument), TROPOMI (Tropospheric Monitoring Instrument), TEMPO (Tropospheric Emissions: Monitoring of Pollution)) measurements of these laminae will observe greater horizontal extent and lower vertical resolution than balloon-borne or lidar measurements will quantify. Using integrated ground-based, airborne, and spaceborne observations in a modeling framework affords insight into how to gain knowledge of both the vertical and horizontal evolution of these ubiquitous ozone laminae.

Tropospheric Ozone↗
NASA NTRS2016

Tropospheric Emissions: Monitoring of Pollution (TEMPO)

TEMPO (Tropospheric Emissions: Monitoring of Pollution) was selected in 2012 by NASA as the first Earth Venture Instrument, for launch between 2018 and 2021. It will measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO observes from Mexico City, Cuba, and the Bahamas to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution (approximately 2.1 kilometers N/S by 4.4 kilometers E/W at 36.5 degrees N, 100 degrees W). TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry, as well as contributing to carbon cycle knowledge. Measurements are made hourly from geostationary (GEO) orbit, to capture the high variability present in the diurnal cycle of emissions and chemistry that are unobservable from current low-Earth orbit (LEO) satellites that measure once per day. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a commercial GEO host spacecraft to provide a modest cost mission that measures the spectra required to retrieve ozone (O3), nitrogen dioxide (NO2), sulfur dioxide (SO2), formaldehyde (H2CO), glyoxal (C2H2O2), bromine monoxide (BrO), IO (iodine monoxide),water vapor, aerosols, cloud parameters, ultraviolet radiation, and foliage properties. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O3 chemistry cycle. Multi-spectral observations provide sensitivity to O3 in the lowermost troposphere, substantially reducing uncertainty in air quality predictions. TEMPO quantifies and tracks the evolution of aerosol loading. It provides these near-real-time air quality products that will be made publicly available. TEMPO will launch at a prime time to be the North American component of the global geostationary constellation of pollution monitoring together with the European Sentinel-4 (S4) and Korean Geostationary Environment Monitoring Spectrometer (GEMS) instruments.

tropospheric measurement suite↗
NASA NTRS2016

Evaluating a Priori Ozone Profile Information Used in TEMPO Tropospheric Ozone Retrievals

Ozone (O3) is a greenhouse gas and toxic pollutant which plays a major role in air quality. Typically, monitoring of surface air quality and O3 mixing ratios is primarily conducted using in situ measurement networks. This is partially due to high-quality information related to air quality being limited from space-borne platforms due to coarse spatial resolution, limited temporal frequency, and minimal sensitivity to lower tropospheric and surface-level O3. The Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite is designed to address these limitations of current space-based platforms and to improve our ability to monitor North American air quality. TEMPO will provide hourly data of total column and vertical profiles of O3 with high spatial resolution to be used as a near-real-time air quality product.TEMPO O3 retrievals will apply the Smithsonian Astrophysical Observatory profile algorithm developed based on work from GOME, GOME-2, and OMI. This algorithm uses a priori O3 profile information from a climatological data-base developed from long-term ozone-sonde measurements (tropopause-based (TB) O3 climatology). It has been shown that satellite O3 retrievals are sensitive to a priori O3 profiles and covariance matrices. During this work we investigate the climatological data to be used in TEMPO algorithms (TB O3) and simulated data from the NASA GMAO Goddard Earth Observing System (GEOS-5) Forward Processing (FP) near-real-time (NRT) model products. These two data products will be evaluated with ground-based lidar data from the Tropospheric Ozone Lidar Network (TOLNet) at various locations of the US. This study evaluates the TB climatology, GEOS-5 climatology, and 3-hourly GEOS-5 data compared to lower tropospheric observations to demonstrate the accuracy of a priori information to potentially be used in TEMPO O3 algorithms. Here we present our initial analysis and the theoretical impact on TEMPO retrievals in the lower troposphere.

TEMPO↗
NASA NTRSDate not supplied

Global Burden of Tropospheric Ozone: Effects of Particulate Nitrate Photolysis and Assimilation of NO2 Measurements

Tropospheric ozone is a major pollutant, a greenhouse gas, and the primary source of the hydroxyl radical. It is largely produced in situ from the oxidation of CO and volatile organic compounds in the presence of nitrogen oxides (NOx=NO+NO2). Global atmospheric chemistry models generally underestimate NOx and CO concentrations in the northern hemisphere away from source regions, which would lead to an underestimate in the tropospheric ozone burden. Here we evaluate the tropospheric ozone simulation in the GEOS-Chem model (version 14) using observations from satellite, aircraft, and ozonesondes. We include GEOS-Chem simulations conducted in the standard offline mode, as well as in the online mode within the NASA GEOS earth system model which forms the basis for the GEOS Composition Forecasts (GEOS-CF). In both configurations, GEOS-Chem underestimates ozone concentrations in the northern midlatitude free troposphere in spring and summer. We find that we can improve the ozone simulation by including an additional NOx source over the oceans from particulate nitrate photolysis on sea salt aerosols at rates inferred from field studies over the Atlantic Ocean. We investigate whether further improvements in the ozone simulation can be achieved by assimilating satellite measurements of NO2 from the Ozone Monitoring Instrument (OMI) and CO from the Measurement of Pollution in the Troposphere (MOPITT) instruments.

tropospheric ozone↗
NASA NTRS1977

Non Urban Troposphere Composition Symposium, Hollywood, Fla., November 10-12, 1976, Proceedings

Papers are presented which originate from a conference on 'The Non-Urban Troposphere Composition', held in 1976. Attention is given to distributions of nitrous oxide in the atmosphere, and to tropospheric and stratospheric compositions which are perturbed by NO(x) emissions from high-altitude aircraft. Ozone is studied in terms of in situ measurements; various meteorological analyses of tropopause folding, ozone measurements in the Boston area, and ozone measurements in rural areas are presented. A one-dimensional model used to study tropospheric photochemistry numerically is presented as are vertical profiles of tropospheric and stratospheric molecular hydrogen. The oxidation of ammonia, methane, and hydrogen sulfide is assessed in nonurban tropospheres along with nonurban measurements of ethane and methane for various atmospheric conditions. With reference to the particle size distribution of chloride in the marine aerosol, organic and inorganic chlorine concentrations are evaluated, and measurements of sea-air CO2 flux by eddy correlation are investigated.

Source record↗
NASA NTRS1978

Parametric modeling of low-frequency water-vapor-induced tropospheric path length fluctuations

Detailed wet tropospheric fluctuation information is presented in support of proposals to search for gravitational waves in ultra-precise Doppler data. The similarities between the solar wind and tropospheric effects on apparent signal path length are used to hypothesize a parametric model for low-frequency wet tropospheric path length fluctuation. Experimental observations of wet tropospheric signal delay fluctuations are interpreted as confirmation of this parametric form. The model is used to suggest the appropriate conditions for collection of experimental tropospheric fluctuation data.

Berman, A. L.↗
NASA NTRS1980

Simultaneous presence of O3 and CO bands in the troposphere

Vertical profiles of CO and O3 in the troposphere and lower stratosphere have been constructed during a series of flights conducted in July and August 1974 over the American continents between 53 deg S and 67 deg N. The mixing ratios of both gases show large fluctuations with altitude in the Northern Hemisphere. Most of the observed bands of O3 in the free troposphere are coexistent with elevated CO concentrations indicating that this O3 is probably not of stratospheric origin, but most likely produced in the troposphere. From the observations, it is not clear whether these high concentrations of ozone were produced in situ in the remote troposphere or had been transported out of a polluted boundary layer. Isentropic trajectory calculations likewise indicate that the air containing these elevated ozone and carbon monoxide concentrations had been situated in the troposphere for at least 72 h prior to being sampled.

Fishman, J.↗
NASA NTRS1980

Iodine - Its possible role in tropospheric photochemistry

A detailed study of the photochemistry of iodine and its oxides indicates that iodine species may play an important role in the tropospheric photochemical system. Methyl iodide, often observed in the marine troposphere with an average concentration of 5-10 ppt, is photolyzed and thereby produces I atoms. Chemical interactions with O3, HxOy, and NOx cause I to be converted to other inorganic compounds such as IO, HOI, IONO2, and I2. The production of these species and their subsequent recycling back to I can lead to the catalytic removal of tropospheric O3, the enhancement of the NO2/NO ratio, the destruction of HxOy free radicals, and the conversion of HO2 to OH. Ultimately, tropospheric inorganic iodine is removed by heterogeneous processes. Calculations using a numerical model to simulate tropospheric photochemistry indicate that iodine may have a strong impact upon the atmospheric O3-NOx-HxOy system. The magnitude of these effects is dependent upon the value of several uncertain rate constants and the primary source distributions of CH3I and other organic and inorganic iodine compounds.

Chameides, W. L.↗
NASA NTRS1981

On the warming of the polar troposphere during the stratospheric warming of January 1977

In January 1977, a warming of the polar troposphere occurred following a major stratospheric warming. The temperature increase in the polar troposphere is found to be larger below 400 mb than in the upper troposphere. Analysis of the heat budget of the polar troposphere shows that the eddy heat flux convergence is the major factor responsible for the tropospheric warming.

Hansen, A. R.↗
NASA NTRS1982

Ammonia and the NOx budget of the troposphere

Liu et al. (1980) suggested that NOx transported from the stratosphere, as opposed to the anthropogenic source of NOx, may be the dominant source that controls the distribution of NOx in the global troposphere. These ideas require a reinvestigation, and, in particular, an assessment of the role of the oxidation of ammonia as a source of NOx. Attention is given to the results of an ammonia measurement program, in which the vertical distribution of ammonia in the troposphere and lower stratosphere could be studied with the aid of the Infrared Heterodyne Radiometer (IHR), a solar-viewing remote sensor. A one-dimensional photochemical model of the troposphere reported by Levine et al. (1980) was employed to study the chemical and physical processes that control the loss of ammonia in the troposphere. The results of the considered investigation suggest that the oxidation of ammonia may indeed be a significant source of NOx in the troposphere.

Levine, J. S.↗
NASA NTRS1982

Airborne lidar investigations of ozone and aerosols in the nonurban troposphere

A description is presented of the first application of an airborne optical radar (lidar) to measurements of ozone and aerosol profiles in regional and global tropospheric investigations. It is pointed out that high spatial resolution measurements of ozone and aerosols are important in studying the relative contribution of chemistry and transport in large scale atmospheric processes. The investigation makes use of an airborne differential absorption optical radar system, which has been developed for the remote profiling of O3 and aerosols in the troposphere. Attention is given to lower tropospheric measurements and upper tropospheric measurements. The obtained results demonstrate the capability of the considered system to measure O3 and aerosol profiles in the troposphere and lower stratosphere.

Browell, E. V.↗