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NASA NTRS2021

Formaldehyde evolution in U.S. wildfire plumes during FIREX-AQ

Formaldehyde (HCHO) is one of the most abundant non-methane volatile organic compounds (VOCs) emitted by fires. HCHO also undergoes chemical production and loss as a fire plume ages, and it can be an important oxidant precursor. In this study, we disentangle the processes controlling HCHO by examining its evolution in wildfire plumes sampled by the NASA DC-8 during the FIREX-AQ field campaign. In nine of the twelve analyzed plumes, dilution-normalized HCHO increases with physical age (range 1 – 6 h). The balance of HCHO loss (mainly via photolysis) and production (via OH-initiated VOC oxidation) seems to control the sign and magnitude of this trend. Plume-average OH concentrations, calculated from VOC decays, range from –0.5 (± 0.5) × 10 6 to 5.3 (±0.7) × 10 6 cm -3 . The production and loss rates of dilution-normalized HCHO seem to decrease with plume age. Plume-to-plume variability in dilution-normalized secondary HCHO production correlates with OH abundance rather than normalized OH reactivity, suggesting that OH is the main driver of fire-to-fire variability in HCHO secondary production. Analysis suggests an effective HCHO yield of 0.33 (± 0.05) per VOC molecule oxidized for the 12 wildfire plumes. This finding can help connect space-based HCHO observations to the oxidizing capacity of the atmosphere and to VOC emissions.

Air quality↗

DOE OSTI2024

Role of chemical production and depositional losses on formaldehyde in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)

Abstract. Formaldehyde (HCHO) is an important air pollutant with direct cancer risk and ozone-forming potential. HCHO sources are complex because HCHO is both directly emitted and produced from oxidation of most gas-phase reactive organic carbon. We update the secondary production of HCHO in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) in the Community Multiscale Air Quality (CMAQ) model. Production of HCHO from isoprene and monoterpenes is increased, correcting an underestimate in the current version. Simulated June–August surface HCHO during peak photochemical production (11:00–15:00 LT, local time) increased by 0.6 ppb (32 %) over the southeastern USA and by 0.2 ppb (13 %) over the contiguous USA. The increased HCHO compares more favorably with satellite-based observations from the TROPOspheric Monitoring Instrument (TROPOMI) and from aircraft-based observations. Evaluation against hourly surface observations indicates a missing nighttime sink that can be improved by increased nighttime deposition, which reduces June–August nocturnal (20:00–04:00 LT) surface HCHO by 1.1 ppb (36 %) over the southeastern USA and 0.5 ppb (29 %) over the contiguous USA. The ability of CRACMM to capture peak levels of HCHO at midday is improved, particularly at sites in the northeastern USA, while peak levels at sites in the southeastern USA are improved, although still lower than observed. Using established risk assessment methods, lifetime exposure of the population in the contiguous USA (∼ 320 million) to ambient HCHO levels predicted here may result in 6200 lifetime cancer cases, with 40 % from controllable anthropogenic emissions of nitrogen oxides and reactive organic compounds. Chemistry updates will be available in CRACMM version 2 (CRACMM2) in CMAQv5.5.

Skipper, T. Nash↗

NASA NTRS2023

Satellite Remote-Sensing Capability to Assess Tropospheric-Column Ratios of Formaldehyde and Nitrogen Dioxide: Case Study During the Long Island Sound Tropospheric Ozone Study 2018 (LISTOS 2018) Field Campaign

Satellite retrievals of tropospheric-column formaldehyde (HCHO) and nitrogen dioxide (NO 2 ) are frequently used to investigate the sensitivity of ozone (O 3 ) production to emissions of nitrogen oxides and volatile organic carbon compounds. This study inter-compared the systematic biases and uncertainties in retrievals of NO 2 and HCHO, as well as resulting HCHO–NO 2 ratios (FNRs), from two commonly applied satellite sensors to investigate O 3 production sensitivities (Ozone Monitoring Instrument, OMI, and TROPOspheric Monitoring Instrument, TROPOMI) using airborne remote-sensing data taken during the Long Island Sound Tropospheric Ozone Study 2018 between 25 June and 6 September 2018. Compared to aircraft-based HCHO and NO 2 observations, the accuracy of OMI and TROPOMI were magnitude-dependent with high biases in clean environments and a tendency towards more accurate comparisons to even low biases in moderately polluted to polluted regions. OMI and TROPOMI NO 2 systematic biases were similar in magnitude (normalized median bias, NMB = 5 %–6 %; linear regression slope ≈ 0.5–0.6), with OMI having a high median bias and TROPOMI resulting in small low biases. Campaign-averaged uncertainties in the three satellite retrievals (NASA OMI; Quality Assurance for Essential Climate Variables, QA4ECV OMI; and TROPOMI) of NO 2 were generally similar, with TROPOMI retrievals having slightly less spread in the data compared to OMI. The three satellite products differed more when evaluating HCHO retrievals. Campaign-averaged tropospheric HCHO retrievals all had linear regression slopes ∼0.5 and NMBs of 39 %, 17 %, 13 %, and 23 % for NASA OMI, QA4ECV OMI, and TROPOMI at finer (0.05° x 0.05°) and coarser (0.15° x 0.15°) spatial resolution, respectively. Campaign-averaged uncertainty values (root mean square error, RMSE) in NASA and QA4ECV OMI HCHO retrievals were ~9.0 x 10 15 molecules cm –2 (∼ 50 %–55 % of mean column abundance), and the higher-spatial-resolution retrievals from TROPOMI resulted in RMSE values ∼30 % lower. Spatially averaging TROPOMI tropospheric-column HCHO, along with NO 2 and FNRs, to resolutions similar to the OMI reduced the uncertainty in these retrievals. Systematic biases in OMI and TROPOMI NO 2 and HCHO retrievals tended to cancel out, resulting in all three satellite products comparing well to observed FNRs. However, while satellite-derived FNRs had minimal campaign-averaged median biases, unresolved errors in the indicator species did not cancel out in FNR calculations, resulting in large RMSE values compared to observations. Uncertainties in HCHO retrievals were determined to drive the unresolved biases in FNR retrievals.

Matthew S. Johnson↗

NASA NTRS2010

The Unique OMI HCHO/NO2 Feature During the 2008 Beijing Summer Olympics: Implications for Ozone Production Sensitivity

In preparation of the Beijing Summer Olympic and Paralympics Games, strict controls were imposed between July and September 2008 on motor vehicle traffic and industrial emissions to improve air quality for the competitors. We assessed chemical sensitivity of ozone production to these controls using Ozone Monitoring Instrument (OMI) column measurements of formaldehyde (HCHO) and nitrogen dioxide (NO2), where their ratio serves as a proxy for the sensitivity. During the emission controls, HCHO/NO2 increased and indicated a NOx-limited regime, in contrast to the same period in the preceding three years when the ratio indicates volatile organic carbon (VOC)-limited and mixed NOx-VOC-limited regimes. After the emission controls were lifted, observed NO2 and HCHO/NO2 returned to their previous values. The 2005-2008 OMI record shows that this transition in regimes was unique as ozone production in Beijing was rarely NOx-limited. OMI measured summertime increases in HCHO of around 13% in 2008 compared to prior years, the same time period during which MODIS vegetation indices increased. The OMI HCHO increase may be due to higher biogenic emissions of HCHO precursors, associated with Beijing's greening initiative for the Olympics. However, NO2 and HCHO were also found to be well-correlated during the summer months. This indicates an anthropogenic VOC contribution from vehicle emissions to OMI HCHO and is a plausible explanation for the relative HCHO minimum observed in August 2008, concurrent with a minimum in traffic emissions. We calculated positive trends in 2005-2008 OMI HCHO and NO2 of about +1 x 10(exp 14) Molec/ square M-2 and +3 x 10(exp 13) molec CM-2 per month, respectively. The positive trend in NO2 may be an indicator of increasing vehicular traffic since 2005, while the positive trend in HCHO may be due to a combined increase in anthropogenic and biogenic emissions since 2005.

Witte, J. C.↗

NASA NTRS2017

Impact of Evolving Isoprene Mechanisms on Simulated Formaldehyde: An Inter-comparison Supported by in Situ Observations from SENEX

Isoprene oxidation schemes vary greatly among gas-phase chemical mechanisms, with potentially significant ramifications for air quality modeling and interpretation of satellite observations in biogenic-rich regions. In this study, in situ observations from the 2013 SENEX mission are combined with a constrained O-D photochemical box model to evaluate isoprene chemistry among five commonly used gas-phase chemical mechanisms: CBO5, CB6r2, MCMv3.2, MCMv3.3.1, and a recent version of GEOS-Chem. Mechanisms are evaluated and inter-compared with respect to formaldehyde (HCHO), a high-yield product of isoprene oxidation. Though underestimated by all considered mechanisms, observed HCHO mixing ratios are best reproduced by MCMv3.3.1 (normalized mean bias = -15%), followed by GEOS-Chem (-17%), MCMv3.2 (-25%), CB6r2 (-32%) and CB05 (-33%). Inter-comparison of HCHO production rates reveals that major restructuring of the isoprene oxidation scheme in the Carbon Bond mechanism increases HCHO production by only approx. 5% in CB6r2 relative to CBO5, while further refinement of the complex isoprene scheme in the Master Chemical Mechanism increases HCHO production by approx. 16% in MCMv3.3.1 relative to MCMv3.2. The GEOS-Chem mechanism provides a good approximation of the explicit isoprene chemistry in MCMv3.3.1 and generally reproduces the magnitude and source distribution of HCHO production rates. We analytically derive improvements to the isoprene scheme in CB6r2 and incorporate these changes into a new mechanism called CB6r2-UMD, which is designed to preserve computational efficiency. The CB6r2-UMD mechanism mimics production of HCHO in MCMv3.3.1 and demonstrates good agreement with observed mixing ratios from SENEX (-14%). Improved simulation of HCHO also impacts modeled ozone: at approx. 0.3 ppb NO, the ozone production rate increases approx. 3% between CB6r2 and CB6r2-UMD, and rises another approx. 4% when HCHO is constrained to match observations.

isoprene↗

NASA NTRS2021

Wintertime Formaldehyde: Airborne Observations and Source Apportionment Over the Eastern United States

Formaldehyde (HCHO) is generated from direct urban emission sources and secondary production from the photochemical reactions of urban smog. HCHO is linked to tropospheric ozone formation, and contributes to the photochemical reactions of other components of urban smog. In this study pollution plume intercepts during the Wintertime INvestigation of Transport, Emissions, and Reactivity (WINTER) campaign were used to investigate and characterize the formation of HCHO in relation to several anthropogenic tracers. Analysis of aircraft intercepts combined with detailed chemical box modeling downwind of several cities suggest that the most important contribution to observed HCHO was primary emission. A box model analysis of a single plume suggested that secondary sources contribute 21±10% of observed HCHO. Ratios of HCHO/CO observed in the northeast U.S., from Ohio to New York, ranging from 0.2-0.6%, are consistent with direct emissions combined with at most modest photochemical production. Analysis of the nocturnal boundary layer and residual layer from repeated vertical profiling over urban influenced areas indicate a direct HCHO emission flux of 1.3 x 10 14 molecules cm -2 h -1 . In a case study in Atlanta, GA, nighttime HCHO exhibited a ratio to CO (0.6 – 1.8%) and was anti-correlated with O 3 . Observations were consistent with mixing between direct HCHO emissions in urban air masses with those influenced by more rapid HCHO photochemical production. The HCHO/CO emissions ratios determined from the measured data are 2.3 - 15 times greater than the NEI 2017 emissions database. The largest observed HCHO/CO was 1.7 – 1.8%, located near co-generating power stations.

Formaldehyde↗

NASA NTRS2025

Validation of Formaldehyde Products From Three Satellite Retrievals (OMI SAO, OMPS-NPP SAO, and OMI BIRA) in the Marine Atmosphere With Four Seasons of Atom Aircraft Observations

Formaldehyde (HCHO) in the atmosphere is an intermediate product from the oxidation of methane and non-methane volatile organic compounds. In remote marine regions, HCHO variability is closely related to atmospheric oxidation capacity and modeled HCHO in these regions is usually added as a global satellite HCHO background. Thus, it is important to understand and validate the levels of satellite HCHO over the remote oceans. Here we intercompare three satellite retrievals of total HCHO columns (OMI-SAO (v004), OMPS-NPP SAO, and OMI BIRA) and validate them against in situ observations from the NASA Atmospheric Tomography Mission (ATom) mission. All retrievals are correlated with ATom integrated columns over remote oceans, with OMI SAO (v004) showing the best agreement. This is also reflected in the mean bias (MB) for OMI SAO (-0.73±0.87) x 10 15 molec cm -2 , OMPS SAO (-0.76±0.88) x 10 15 molec cm -2 , and OMI BIRA (-1.40±1.11) x 10 15 molec cm -2 . We recommend the OMI-SAO (v004) retrieval for remote ocean atmosphere studies. Three satellite HCHO retrievals and in situ ATom columns all generally captured the spatial and seasonal distributions of HCHO in the remote ocean atmosphere. Retrieval bias varies by latitude and season, but a persistent low bias is found in all products at high latitudes and the general low bias is most severe for the OMI BIRA product. Examination of retrieval components reveals slant column corrections have a larger impact on the retrievals over remote marine regions while AMFs play a smaller role. This study informs that the potential latitude-dependent biases in the retrievals require further investigation for improvement and should be considered when using marine HCHO satellite data, and vertical profiles from in situ instruments are crucial for validating satellite retrievals.

Atom↗

NASA NTRS1984

Importance of formaldehyde in cloud chemistry

A physical-chemical model which is an extension of that of Hong and Carmichael (1983) is used to investigate the role of formaldehyde in cloud chemistry. This model takes into account the mass transfer of SO2, O3, NH3, HNO3, H2O2, CO2, HCl, HCHO, O2, OH and HO2 into cloud droplets and their subsequent chemical reactions. The model is used to assess the importance of S(IV)-HCHO adduct formation, the reduction of H2O2 by HCHO, HCHO-free radical interactions, and the formation of HCOOH in the presence of HCHO in cloud droplets. Illustrative calculations indicate that the presence of HCHO inhibits sulfate production rate in cloud droplets. The direct inhibition of sulfate production rate in cloudwater due to nucleophilic addition of HSO3(-) to HCHO(aq) to form hydroxymethanesulfonate is generally low for concentrations of HCHO typical of ambient air. However, inhibition of sulfate production due to formaldehyde-free radical interactions in solution can be important. These formaldehyde-free radical reactions can also generate appreciable quantities of formic acid.

Adewuyi, Y. G.↗

NASA NTRS2004

Mapping Isoprene Emissions over North America using Formaldehyde Column Observations from Space

I] We present a methodology for deriving emissions of volatile organic compounds (VOC) using space-based column observations of formaldehyde (HCHO) and apply it to data from the Global Ozone Monitoring Experiment (GOME) satellite instrument over North America during July 1996. The HCHO column is related to local VOC emissions, with a spatial smearing that increases with the VOC lifetime. lsoprene is the dominant HCHO precursor over North America in summer, and its lifetime (approx. = 1 hour) is sufficiently short that the smearing can be neglected. We use the Goddard Earth Observing System global 3-D model of tropospheric chemistry (GEOS-CHEM) to derive the relationship between isoprene emissions and HCHO columns over North America and use these relationships to convert the GOME HCHO columns to isoprene emissions. We also use the GEOS-CHEM model as an intermediary to validate the GOME HCHO column measurements by comparison with in situ observations. The GEOS-CHEM model including the Global Emissions Inventory Activity (GEIA) isoprene emission inventory provides a good simulation of both the GOME data (r(sup 2) = 0.69, n = 756, bias = +l1 %) and the in situ summertime HCHO measurements over North America (r(sup 2) = 0.47, n = 10, bias = -3%). The GOME observations show high values over regions of known high isoprene emissions and a day-to-day variability that is consistent with the temperature dependence of isoprene emission. Isoprene emissions inferred from the GOME data are 20% less than GEIA on average over North America and twice those from the U S . EPA Biogenic Emissions Inventory System (BEIS2) inventory. The GOME isoprene inventory when implemented in the GEOS-CHEM model provides a better simulation of the HCHO in situ measurements thaneitherGEIAorBEIS2 (r(sup 2) = 0.71,n= 10, bias = -10 %).

Palmer, Paul I.↗

NASA NTRS2017

A New Non-Resonant Laser-Induced Fluorescence Instrument for the Airborne in Situ Measurement of Formaldehyde

A new in situ instrument for gas-phase formaldehyde (HCHO), COmpact Formaldehyde FluorescencE Experiment (COFFEE), is presented. COFFEE utilizes nonresonant laser-induced fluorescence (NR-LIF) to measure HCHO, with 300 mW of 40 kHz 355 nm laser output exciting multiple HCHO absorption features. The resulting HCHO fluorescence is collected at 5 ns resolution, and the fluorescence time profile is fit to yield the ambient HCHO mixing ratio. Typical 1 sigma precision at approximately 0 pptv HCHO is 150 pptv for 1 s data. The compact instrument was designed to operate with minimal in-flight operator interaction and infrequent maintenance (1-2 times per year). COFFEE fits in the wing pod of the Alpha Jet stationed at the NASA Ames Research Center and has successfully collected HCHO data on 27 flights through 2017 March. The frequent flights, combined with a potentially long-term data set, makes the Alpha Jet a promising platform for validation of satellite-based column HCHO.

Nonresonant laser-induced fluorescenc↗

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 NTRS2020

Revisiting the Effectiveness Of HCHO/NO2 Ratios for Inferring Ozone Sensitivity to Its Precursors Using High Resolution Airborne Remote Sensing Observations in A High Ozone Episode During the KORUS-AQ Campaign

The nonlinear chemical processes involved in ozone production (P(O3)) have necessitated using proxy indicators to convey information about the primary dependence of P(O3) on volatile organic compounds (VOCs) or nitrogen oxides (NOx). In particular, the ratio of remotely sensed columns of formaldehyde (HCHO) to nitrogen dioxide (NO2) has been widely used for studying O3 sensitivity. Previous studies found that the errors in retrievals and the incoherent relationship between the column and the near-surface concentrations are a barrier in applying the ratio in a robust way. In addition to these obstacles, we provide calculational-observational evidence, using an ensemble of 0-D photochemical box models constrained by DC-8 aircraft measurements on an ozone event during the Korea-United States Air Quality (KORUS-AQ) campaign over Seoul, to demonstrate the chemical feedback of NO2 on the formation of HCHO is a controlling factor for the transition line between NOx-sensitive and NOx-saturated regimes. A fixed value (~2.7) of the ratio of the chemical loss of NOx (LNOx) to the chemical loss of HO2+RO2 (LROx) perceptibly differentiates the regimes. Following this value, data points with a ratio of HCHO/NO2 less than 1 can be safely classified as NOx-saturated regime, whereas points with ratios between 1 and 4 fall into one or the other regime. We attribute this mainly to the HCHO-NO2 chemical relationship causing the transition line to occur at larger (smaller) HCHO/NO2 ratios in VOC-rich (VOC-poor) environments. We then redefine the transition line to LNOx/LROx~2.7 that accounts for the HCHO-NO2 chemical relationship leading to HCHO = 3.7 × (NO2 – 1.14 × 1016 molec.cm-2). Although the revised formula is locally calibrated (i.e., requires for readjustment for other regions), its mathematical format removes the need for having a wide range of thresholds used in HCHO/NO2 ratios that is a result of the chemical feedback. Therefore, to be able to properly take the chemical feedback into consideration, the use of HCHO = a × (NO2 – b) formula should be preferred to the ratio in future works. We then use the Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) airborne instrument to study O3 sensitivity in Seoul. The unprecedented spatial (250 × 250 m2) and temporal (~every 2 h) resolutions of HCHO and NO2 observations form the sensor enhance our understanding of P(O3) in Seoul; rather than providing a crude label for the entire city, more in-depth variabilities in chemical regimes are observed that should be able to inform mitigation strategies correspondingly.

KORUS-AQ; formaldehyde; NOx; VOC; OMI; GeoTASO; oz↗

NASA NTRS2006

Quantifying the Seasonal and Interannual Variability of North American Isoprene Emissions Using Satellite Observations of the Formaldehyde Column

Quantifying isoprene emissions using satellite observations of the formaldehyde (HCHO) columns is subject to errors involving the column retrieval and the assumed relationship between HCHO columns and isoprene emissions, taken here from the GEOS-CHEM chemical transport model. Here we use a 6-year (1996-2001) HCHO column data set from the Global Ozone Monitoring Experiment (GOME) satellite instrument to (1) quantify these errors, (2) evaluate GOME-derived isoprene emissions with in situ flux measurements and a process-based emission inventory (Model of Emissions of Gases and Aerosols from Nature, MEGAN), and (3) investigate the factors driving the seasonal and interannual variability of North American isoprene emissions. The error in the GOME HCHO column retrieval is estimated to be 40%. We use the Master Chemical Mechanism (MCM) to quantify the time-dependent HCHO production from isoprene, alpha- and beta-pinenes, and methylbutenol and show that only emissions of isoprene are detectable by GOME. The time-dependent HCHO yield from isoprene oxidation calculated by MCM is 20-30% larger than in GEOS-CHEM. GOME-derived isoprene fluxes track the observed seasonal variation of in situ measurements at a Michigan forest site with a -30% bias. The seasonal variation of North American isoprene emissions during 2001 inferred from GOME is similar to MEGAN, with GOME emissions typically 25% higher (lower) at the beginning (end) of the growing season. GOME and MEGAN both show a maximum over the southeastern United States, but they differ in the precise location. The observed interannual variability of this maximum is 20-30%, depending on month. The MEGAN isoprene emission dependence on surface air temperature explains 75% of the month-to-month variability in GOME-derived isoprene emissions over the southeastern United States during May-September 1996-2001.

Palmer, Paul I.↗

NASA NTRS2016

Airborne In-Situ Measurements of Formaldehyde Over California: First Results from the Compact Formaldehyde Fluorescence Experiment (COFFEE) Instrument

Formaldehyde (HCHO) is one of the most abundant oxygenated volatile organic compounds (VOCs) in the atmosphere, playing a role multiple atmospheric processes. Measurements of HCHO can be used to help quantify convective transport, the abundance of VOCs, and ozone production in urban environments. The Compact Formaldehyde FluorescencE Experiment (COFFEE) instrument uses Non-Resonant Laser Induced Fluorescence (NR-LIF) to detect trace concentrations of HCHO as part of the Alpha Jet Atmospheric eXperiment (AJAX) payload. Developed at NASA GSFC, COFFEE is a small, low maintenance instrument with a sensitivity of 100 pptv and a quick response time (1 sec). The COFFEE instrument has been customized to fit in an external wing pod on the Alpha Jet aircraft based at NASA ARC. The instrument can operate over a broad range of altitudes, from boundary layer to lower stratosphere, making it well suited for the Alpha Jet, which can access altitudes from the surface up to 40,000 ft. Results of the first COFFEE science flights preformed over the California's Central Valley will be presented. Boundary layer measurements and vertical profiles in the tropospheric column will both be included. This region is of particular interest, due to its elevated levels of HCHO, revealed in satellite images, as well as its high ozone concentrations. In addition to HCHO, the AJAX payload includes measurements of atmospheric ozone, methane, and carbon dioxide. Formaldehyde is one of the few urban pollutants that can be measured from space. Plans to compare in-situ COFFEE data with satellite-based HCHO observations such as those from OMI (Aura) and OMPS (SuomiNPP) will also be presented.

ozone↗

NASA NTRS2016

Airborne In-Situ Measurements of Formaldehyde over California: First Results from the Compact Formaldehyde Fluorescence Experiment (COFFEE) Instrument

coffee↗

NASA NTRS2017

Glyoxal Yield from Isoprene Oxidation and Relation to Formaldehyde: Chemical Mechanism, Constraints from SENEX Aircraft Observations, and Interpretation of OMI Satellite Data

Glyoxal (CHOCHO) is produced in the atmosphere by the oxidation of volatile organic compounds(VOCs). Like formaldehyde (HCHO), another VOC oxidation product, it is measurable from space by solar backscatter. Isoprene emitted by vegetation is the dominant source of CHOCHO and HCHO in most of the world. We use aircraft observations of CHOCHO and HCHO from the Southeast Nexus (SENEX) campaign over the southeast US in summer 2013 to better understand the CHOCHO time-dependent yield from isoprene oxidation, its dependence on nitrogen oxides (NO (sub x) triple bonded to NO plus NO2), the behavior of the CHOCHO-HCHO relationship, the quality of Ozone Monitoring Instrument (OMI) CHOCHO satellite observations, and the implications for using CHOCHO observations from space as constraints on isoprene emissions. We simulate the SENEX and OMI observations with the Goddard Earth Observing System chemical transport model (GEOSChem) featuring a new chemical mechanism for CHOCHO formation from isoprene. The mechanism includes prompt CHOCHO formation under low-NO (sub x) conditions following the isomerization of the isoprene peroxy radical (ISOPO2).The SENEX observations provide support for this prompt CHOCHO formation pathway, and are generally consistent with the GEOS-Chem mechanism. Boundary layer CHOCHO and HCHO are strongly correlated in the observations and the model, with some departure under low-NO (sub x) conditions due to prompt CHOCHO formation. SENEX vertical profiles indicate a free-tropospheric CHOCHO background that is absent from the model. The OMI CHOCHO data provide some support for this free-tropospheric background and show southeast US enhancements consistent with the isoprene source but a factor of 2 too low. Part of this OMI bias is due to excessive surface reflectivities assumed in the retrieval. The OMI CHOCHO and HCHO seasonal data over the southeast US are tightly correlated and provide redundant proxies of isoprene emissions. Higher temporal resolution in future geostationary satellite observations may enable detection of the prompt CHOCHO production under low-NO (sub x) conditions apparent in the SENEX data.

OMI↗

NASA NTRS2016

Airborne In-Situ Measurements of Formaldehyde Over California: One Year of Results from the Compact Formaldehyde Fluorescence Experiment (COFFEE) Instrument

Formaldehyde (HCHO) is one of the most abundant oxygenated volatile organiccompounds (VOCs) in the atmosphere, playing a role in multiple atmosphericprocesses, such as ozone (O3) production in polluted environments. Due toits short lifetime of only a few hours in daytime, HCHO also serves astracer of recent photochemical activity. While photochemical oxidation ofnon-methane hydrocarbons is the dominant source, HCHO can also be emitteddirectly from fuel combustion, vegetation, and biomass burning. The CompactFormaldehyde FluorescencE Experiment (COFFEE) instrument was built forintegration onto the Alpha Jet Atmospheric eXperiment (AJAX) payload, basedout of NASAs Ames Research Center (Moffett Field, CA). Using Non-ResonantLaser Induced Fluorescence (NR-LIF), trace concentrations of HCHO can bedetected with a sensitivity of 200 parts per trillion.Since its first research flight in December 2015, COFFEE has successfullyflown on more than 20 science missions throughout California and Nevada.Presented here are results from these flights, including boundary layermeasurements and vertical profiles throughout the tropospheric column.Californias San Joaquin Valley is a primary focus, as this region is knownfor its elevated levels of HCHO as well as O3. Measurements collected inwildfire plumes, urban centers, agricultural lands, and on and off shorecomparisons will be presented. In addition, the correlation of HCHO to othertrace gases also measured by AJAX, including O3, methane, carbon dioxide,and water vapor will also be shown. Lastly, the implications of these HCHOmeasurements on calibration and validation of remote sensing data collectedby NASAs OMI (Aura) and OMPS (SuomiNPP) satellites will be addressed.

wildfire↗

NASA NTRS2019

Explicit Aerosol Correction of OMI Formaldehyde Retrievals

Atmospheric aerosols are significant sources of uncertainty in air mass factor (AMF) calculations for trace gas retrievals using ultraviolet measurements from space. Current trace gas retrievals typically do not consider aerosols explicitly as cloud products partially account for aerosol effects. Here, we propose a new measurement-based approach to correct for aerosols explicitly in the AMF calculation, apply it to Ozone Monitoring Instrument (OMI) formaldehyde (HCHO) retrievals and quantify the aerosol-induced HCHO vertical column density difference for three aerosol types (smoke, dust, and sulfate) during 2006–2007. We use OMI aerosol retrievals for aerosol optical properties and vertical profiles to construct lookup tables of scattering weights as functions of geometry, surface pressure, surface albedo, and aerosol information. The average difference between the National Aeronautics and Space Administration operational OMI HCHO product (not considering aerosols) and the results obtained in this study on a global scale are 27%, 6%, and −0.3% for smoke, dust, and sulfate aerosols, respectively. The region with the largest aerosol effects is East China, where the explicit smoke aerosol correction enhances mean HCHO vertical column densities by 35%, with corrections to individual observations sometimes larger than 100%. The quantified aerosol effects are applicable under clear-sky conditions. This study highlights the need to implement aerosol corrections in the AMF calculation for HCHO retrievals. This is particularly relevant in regions with high levels of pollution where aerosols interfere the most with formaldehyde satellite observations.

Ozone Monitoring Instrument (OMI) formaldehyde (HC↗