Air pollution monitoring using mobile ground-based measurement platforms can provide high quality spatiotemporal air pollution information. As mobile air quality monitoring campaigns extend to entire fleets of vehicles and integrate smaller scale air quality sensors, it is important to address the need for assessing these measurements in a scalable manner. We explore collocation-based evaluation of air quality measurements in a mobile platform using fixed regulatory sites as a reference. We compare two approaches - a standard collocation assessment technique where the mobile platform is parked near the fixed regulatory site for a period of time and an expanded approach using measurements while the mobile platform is in motion in the general vicinity of the fixed regulatory site. Based on the availability of fixed reference site data, we focus on three pollutants (ozone, nitrogen dioxide, and nitric oxide) with distinct atmospheric lifetimes and behaviors. We compare measurements from a mobile laboratory with regulatory site measurements in Denver, Colorado, USA and in the San Francisco Bay Area, California, USA. Our one-month Denver dataset includes both parked collocation periods near the fixed regulatory sites as well as general driving patterns around the sites, allowing a direct comparison of the parked and mobile collocation techniques on the same dataset. We show that the mobile collocation approach produces similar performance statistics, including coefficients of determination and mean bias errors, as the standard parked collocation technique. This is particularly true when the comparisons are restricted to specific road types, with residential streets showing the closest agreement and highways showing the largest differences. We extend our analysis to a larger (year-long) dataset in California, where we explore the relationships between the mobile measurements and the fixed reference sites on a larger scale. We show that using a 40-hour running median converges to within ±4 ppbv of the fixed reference site for nitrogen dioxide and ozone and up to about 8 ppbv for nitric oxide. We propose that this agreement can be leveraged to assess instrument performance over time during large-scale mobile monitoring campaigns. We demonstrate an example of how such relationships can be used during large-scale monitoring campaigns using small sensors to identify potential measurement biases.

Globally, billions of people burn fuels indoors for cooking and heating, which contributes to millions of chronic illnesses and premature deaths annually. Additionally, residential burning contributes significantly to black carbon emissions, which have the highest global warming impacts after carbon dioxide and methane. In this study, we use Fourier transform infrared spectroscopy (FTIR) to analyze fine-particulate emissions collected on Teflon membrane filters from 15 cookstove types and 5 fuel types. Emissions from three fuel types (charcoal, kerosene, and red oak wood) were found to have enough FTIR spectral response for functional group (FG) analysis. We present distinct spectral profiles for particulate emissions of these three fuel types. We highlight the influential FGs constituting organic carbon (OC) using a multivariate statistical method and show that OC estimates by collocated FTIR and thermal-optical transmittance (TOT) are highly correlated, with a coefficient determination of 82.5 %. As FTIR analysis is fast and non-destructive and provides complementary FG information, the analysis method demonstrated herein can substantially reduce the need for thermal-optical measurements for source emissions.

PurpleAir sensors, which measure particulate matter (PM), are widely used by individuals, community groups, and other organizations including state and local air monitoring agencies. PurpleAir sensors comprise a massive global network of more than 10,000 sensors. Previous performance evaluations have typically studied a limited number of PurpleAir sensors in small geographic areas or laboratory environments. While useful for determining sensor behavior and data normalization for these geographic areas, little work has been done to understand the broad applicability of these results outside these regions and conditions. Here, PurpleAir sensors operated by air quality monitoring agencies are evaluated in comparison to collocated ambient air quality regulatory instruments. In total, almost 12,000 24-hour averaged PM measurements from collocated PurpleAir sensors and Federal Reference Method (FRM) or Federal Equivalent Method (FEM) PM measurements were collected across diverse regions of the United States (U.S.), including 16 states. Consistent with previous evaluations, under typical ambient and smoke impacted conditions, the raw data from PurpleAir sensors overestimate PM concentrations by about 40% in most parts of the U.S. A simple linear regression reduces much of this bias across most U.S. regions, but adding a relative humidity term further reduces the bias and improves consistency in the biases between different regions. More complex multiplicative models did not substantially improve results when tested on an independent dataset. The final PurpleAir correction reduces the root mean square error (RMSE) of the raw data from 8 μg m to 3 μg m with an average FRM or FEM concentration of 9 μg m. This correction equation, along with proposed data cleaning criteria, has been applied to PurpleAir PM measurements across the U.S. in the AirNow Fire and Smoke Map (fire.airnow.gov) and has the potential to be successfully used in other air quality and public health applications.

In recent years wildland fires in the United States have had significant impacts on local and regional air quality and negative human health outcomes. Although the primary health concerns from wildland fires come from fine particulate matter (PM), large increases in ozone (O) have been observed downwind of wildland fire plumes (DeBell et al., 2004; Bytnerowicz et al., 2010; Preisler et al., 2010; Jaffe et al., 2012; Bytnerowicz et al., 2013; Jaffe et al., 2013; Lu et al., 2016; Lindaas et al., 2017; McClure and Jaffe, 2018; Liu et al., 2018; Baylon et al., 2018; Buysse et al., 2019). Conditions generated in and around wildland fire plumes, including the presence of interfering chemical species, can make the accurate measurement of O concentrations using the ultraviolet (UV) photometric method challenging if not impossible. UV photometric method instruments are prone to interferences by volatile organic compounds (VOCs) that are present at high concentrations in wildland fire smoke. Four different O measurement methodologies were deployed in a mobile sampling platform downwind of active prescribed grassland fire lines in Kansas and Oregon and during controlled chamber burns at the United States Forest Service, Rocky Mountain Research Station Fire Sciences Laboratory in Missoula, Montana. We demonstrate that the Federal Reference Method (FRM) nitric oxide (NO) chemiluminescence monitors and Federal Equivalent Method (FEM) gas-phase (NO) chemical scrubber UV photometric O monitors are relatively interference-free, even in near-field combustion plumes. In contrast, FEM UV photometric O monitors using solid-phase catalytic scrubbers show positive artifacts that are positively correlated with carbon monoxide (CO) and total gas-phase hydrocarbon (THC), two indicator species of biomass burning. Of the two catalytic scrubber UV photometric methods evaluated, the instruments that included a Nafion® tube dryer in the sample introduction system had artifacts an order of magnitude smaller than the instrument with no humidity correction. We hypothesize that Nafion®-permeating VOCs (such as aromatic hydrocarbons) could be a significant source of interference for catalytic scrubber UV photometric O monitors and that the inclusion of a Nafion® tube dryer assists with the mitigation of these interferences. The chemiluminescence FRM method is highly recommended for accurate measurements of O in wildland fire plume studies and at regulatory ambient monitoring sites frequently impacted by wildland fire smoke.

Aerial emission sampling of four natural gas boiler stack plumes was conducted using an unmanned aerial system (UAS) equipped with a lightweight sensor-sampling system (the "Kolibri") for measurement of nitrogen oxide (NO), and nitrogen dioxide (NO), carbon dioxide (CO), and carbon monoxide (CO). Flights (=22) ranged from 11 to 24min in duration at two different sites. The UAS was maneuvered into the plumes with the aid of real-time CO telemetry to the ground operators and, at one location, a second UAS equipped with an infrared-visible camera. Concentrations were collected and recorded at 1Hz. The maximum CO, CO, NO, and NO concentrations in the plume measured were 10000, 7, 27, and 1.5 ppm, respectively. Comparison of the NO emissions between the stack continuous emission monitoring systems and the UAS-Kolibri for three boiler sets showed an average of 5.6% and 3.5% relative difference for the run-weighted and carbon-weighted average emissions, respectively. To our knowledge, this is the first evidence of the accuracy performance of UAS-based emission factors against a source of known strength.

The distribution and dynamics of atmospheric pollutants are spatiotemporally heterogeneous due to variability in emissions, transport, chemistry, and deposition. To understand these processes at high spatiotemporal resolution and their implications for air quality and personal exposure, we present custom, low-cost air quality monitors that measure concentrations of contaminants relevant to human health and climate, including gases (e.g., O, NO, NO, CO, CO, CH, and SO) and size-resolved (0.3-10 μm) particulate matter. The devices transmit sensor data and location via cellular communications and are capable of providing concentration data down to second-level temporal resolution. We produce two models: one designed for stationary (or mobile platform) operation and a wearable, portable model for directly measuring personal exposure in the breathing zone. To address persistent problems with sensor drift and environmental sensitivities (e.g., relative humidity and temperature), we present the first online calibration system designed specifically for low-cost air quality sensors to calibrate zero and span concentrations at hourly to weekly intervals. Monitors are tested and validated in a number of environments across multiple outdoor and indoor sites in New Haven, CT; Baltimore, MD; and New York City. The evaluated pollutants (O, NO, NO, CO, CO, and PM) performed well against reference instrumentation (e.g., = 0.66-0.98) in urban field evaluations with fast -folding response times (≤1 min), making them suitable for both large-scale network deployments and smaller-scale targeted experiments at a wide range of temporal resolutions. We also provide a discussion of best practices on monitor design, construction, systematic testing, and deployment.

Airborne and ground-based Pandora spectrometer NO column measurements were collected during the 2018 Long Island Sound Tropospheric Ozone Study (LISTOS) in the New York City/Long Island Sound region, which coincided with early observations from the Sentinel-5P TROPOspheric Monitoring Instrument (TROPOMI) instrument. Both airborne- and ground-based measurements are used to evaluate the TROPOMI NO Tropospheric Vertical Column (TrVC) product v1.2 in this region, which has high spatial and temporal heterogeneity in NO. First, airborne and Pandora TrVCs are compared to evaluate the uncertainty of the airborne TrVC and establish the spatial representativeness of the Pandora observations. The 171 coincidences between Pandora and airborne TrVCs are found to be highly correlated ( =0.92 and slope of 1.03), with the largest individual differences being associated with high temporal and/or spatial variability. These reference measurements (Pandora and airborne) are complementary with respect to temporal coverage and spatial representativity. Pandora spectrometers can provide continuous long-term measurements but may lack areal representativity when operated in direct-sun mode. Airborne spectrometers are typically only deployed for short periods of time, but their observations are more spatially representative of the satellite measurements with the added capability of retrieving at subpixel resolutions of 250m×250m over the entire TROPOMI pixels they overfly. Thus, airborne data are more correlated with TROPOMI measurements ( = 0.96) than Pandora measurements are with TROPOMI ( = 0.84). The largest outliers between TROPOMI and the reference measurements appear to stem from too spatially coarse a priori surface reflectivity (0.5°) over bright urban scenes. In this work, this results during cloud-free scenes that, at times, are affected by errors in the TROPOMI cloud pressure retrieval impacting the calculation of tropospheric air mass factors. This factor causes a high bias in TROPOMI TrVCs of 4%-11%. Excluding these cloud-impacted points, TROPOMI has an overall low bias of 19%-33% during the LISTOS timeframe of June-September 2018. Part of this low bias is caused by coarse a priori profile input from the TM5-MP model; replacing these profiles with those from a 12 km North American Model-Community Multiscale Air Quality (NAMCMAQ) analysis results in a 12%-14% increase in the TrVCs. Even with this improvement, the TROPOMI-NAMCMAQ TrVCs have a 7%-19% low bias, indicating needed improvement in a priori assumptions in the air mass factor calculation. Future work should explore additional impacts of a priori inputs to further assess the remaining low biases in TROPOMI using these datasets.

NASA's Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ, conducted in 2011-2014) campaign in the United States and the joint NASA and National Institute of Environmental Research (NIER) Korea-United States Air Quality Study (KORUS-AQ, conducted in 2016) in South Korea were two field study programs that provided comprehensive, integrated datasets of airborne and surface observations of atmospheric constituents, including nitrogen dioxide (NO), with the goal of improving the interpretation of spaceborne remote sensing data. Various types of NO measurements were made, including in situ concentrations and column amounts of NO using ground- and aircraft-based instruments, while NO column amounts were being derived from the Ozone Monitoring Instrument (OMI) on the Aura satellite. This study takes advantage of these unique datasets by first evaluating in situ data taken from two different instruments on the same aircraft platform, comparing coincidently sampled profile-integrated columns from aircraft spirals with remotely sensed column observations from ground-based Pandora spectrometers, intercomparing column observations from the ground (Pandora), aircraft (in situ vertical spirals), and space (OMI), and evaluating NO simulations from coarse Global Modeling Initiative (GMI) and high-resolution regional models. We then use these data to interpret observed discrepancies due to differences in sampling and deficiencies in the data reduction process. Finally, we assess satellite retrieval sensitivity to observed and modeled a priori NO profiles. Contemporaneous measurements from two aircraft instruments that likely sample similar air masses generally agree very well but are also found to differ in integrated columns by up to 31.9 %. These show even larger differences with Pandora, reaching up to 53.9 %, potentially due to a combination of strong gradients in NO fields that could be missed by aircraft spirals and errors in the Pandora retrievals. OMI NO values are about a factor of 2 lower in these highly polluted environments due in part to inaccurate retrieval assumptions (e.g., a priori profiles) but mostly to OMI's large footprint (> 312 km).

The Cloud-Aerosol Transport System (CATS) lidar on board the International Space Station (ISS) operated from 10 February 2015 to 30 October 2017 providing range-resolved vertical backscatter profiles of Earth's atmosphere at 1064 and 532 nm. The CATS instrument design and ISS orbit lead to a higher 1064 nm signal-to-noise ratio than previous space-based lidars, allowing for direct atmospheric calibration of the 1064 nm signals. Nighttime CATS Version 3-00 data were calibrated by scaling the measured data to a model of the expected atmospheric backscatter between 22 and 26 km above mean sea level (AMSL). The CATS atmospheric model is constructed using molecular backscatter profiles derived from Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) re-analysis data and aerosol scattering ratios measured by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). The nighttime normalization altitude region was chosen to simultaneously minimize aerosol loading and variability within the CATS data frame, which extends from 28 km to -2 km AMSL. Daytime CATS Version 3-00 data were calibrated through comparisons with nighttime measurements of the layer integrated attenuated total backscatter (iATB) from strongly scattering, rapidly attenuating opaque cirrus clouds. The CATS nighttime 1064 nm attenuated total backscatter (ATB) uncertainties for clouds and aerosols are primarily related to the uncertainties in the CATS nighttime calibration technique, which are estimated to be ~9%. Median CATS V3-00 1064 nm ATB relative uncertainty at night within cloud and aerosol layers is 7%, slightly lower than these calibration uncertainty estimates. CATS median daytime 1064 nm ATB relative uncertainty is 21% in cloud and aerosol layers, similar to the estimated 16-18% uncertainty in the CATS daytime cirrus cloud calibration transfer technique. Coincident daytime comparisons between CATS and the Cloud Physics Lidar (CPL) during the CATS-CALIPSO Airborne Validation Experiment (CCAVE) project show good agreement in mean ATB profiles for clear-air regions. Eight nighttime comparisons between CATS and the Polly ground based lidars also show good agreement in clear-air regions between 3-12 km, with CATS having a mean ATB of 19.7 % lower than Polly. Agreement between the two instruments (~7%) is even better within an aerosol layer. Six-month comparisons of nighttime ATB values between CATS and the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) also show that iATB comparisons of opaque cirrus clouds agree to within 19%. Overall, CATS has demonstrated that direct calibration of the 1064 nm channel is possible from a space based lidar using the atmospheric normalization technique.

In this work, a new commercially available, laser-based, and ultra-portable formaldehyde (HCHO) gas sensor is characterized, and its usefulness for monitoring HCHO mixing ratios in both indoor and outdoor environments is assessed. Stepped calibrations and intercomparison with well-established laser-induced fluorescence (LIF) instrumentation allow a performance evaluation of the absorption-based, mid-infrared HCHO sensor from Aeris Technologies, Inc. The Aeris sensor displays linear behavior (R > 0.940) when compared with LIF instruments from Harvard and NASA Goddard. A non-linear least-squares fitting algorithm developed independently of the sensor's manufacturer to fit the sensor's raw absorption data during post-processing further improves instrument performance. The 3σ limit of detection (LOD) for 2, 15, and 60 min integration times are 2190, 690, and 420 pptv HCHO, respectively, for mixing ratios reported in real-time, though the LOD improves to 1800, 570, and 300 pptv HCHO, respectively, during post-processing. Moreover, the accuracy of the sensor was found to be ±(10% + 0.3) ppbv when compared against LIF instrumentation sampling ambient air. This sub-ppbv precision and level of accuracy are sufficient for most HCHO levels measured in indoor and outdoor environments. While the compact Aeris sensor is currently not a replacement for the most sensitive research-grade instrumentation available, its usefulness for monitoring HCHO is clearly demonstrated.

NASA deployed the GeoTASO airborne UV-Visible spectrometer in May-June 2017 to produce high resolution (approximately 250 × 250 m) gapless NO datasets over the western shore of Lake Michigan and over the Los Angeles Basin. The results collected show that the airborne tropospheric vertical column retrievals compare well with ground-based Pandora spectrometer column NO observations (r=0.91 and slope of 1.03). Apparent disagreements between the two measurements can be sensitive to the coincidence criteria and are often associated with large local variability, including rapid temporal changes and spatial heterogeneity that may be observed differently by the sunward viewing Pandora observations. The gapless mapping strategy executed during the 2017 GeoTASO flights provides data suitable for averaging to coarser areal resolutions to simulate satellite retrievals. As simulated satellite pixel area increases to values typical of TEMPO, TROPOMI, and OMI, the agreement with Pandora measurements degraded, particularly for the most polluted columns as localized large pollution enhancements observed by Pandora and GeoTASO are spatially averaged with nearby less-polluted locations within the larger area representative of the satellite spatial resolutions (aircraft-to-Pandora slope: TEMPO scale=0.88; TROPOMI scale=0.77; OMI scale=0.57). In these two regions, Pandora and TEMPO or TROPOMI have the potential to compare well at least up to pollution scales of 30×10 molecules cm. Two publicly available OMI tropospheric NO retrievals are both found to be biased low with respect to these Pandora observations. However, the agreement improves when higher resolution a priori inputs are used for the tropospheric air mass factor calculation (NASA V3 Standard Product slope = 0.18 and Berkeley High Resolution Product slope=0.30). Overall, this work explores best practices for satellite validation strategies with Pandora direct-sun observations by showing the sensitivity to product spatial resolution and demonstrating how the high spatial resolution NO data retrieved from airborne spectrometers, such as GeoTASO, can be used with high temporal resolution ground-based column observations to evaluate the influence of spatial heterogeneity on validation results.

Low-cost sensors for measuring particulate matter (PM) offer the ability to understand human exposure to air pollution at spatiotemporal scales that have previously been impractical. However, such low-cost PM sensors tend to be poorly characterized, and their measurements of mass concentration can be subject to considerable error. Recent studies have investigated how individual factors can contribute to this error, but these studies are largely based on empirical comparisons and generally do not examine the role of multiple factors simultaneously. Here, we present a new physics-based framework and open-source software package () for evaluating the ability of low-cost optical particle sensors (optical particle counters and nephelometers) to accurately characterize the size distribution and/or mass loading of aerosol particles. This framework, which uses Mie theory to calculate the response of a given sensor to a given particle population, is used to estimate the fractional error in mass loading for different sensor types given variations in relative humidity, aerosol optical properties, and the underlying particle size distribution. Results indicate that such error, which can be substantial, is dependent on the sensor technology (nephelometer vs. optical particle counter), the specific parameters of the individual sensor, and differences between the aerosol used to calibrate the sensor and the aerosol being measured. We conclude with a summary of likely sources of error for different sensor types, environmental conditions, and particle classes and offer general recommendations for the choice of calibrant under different measurement scenarios.

Mobile platform measurements provide new opportunities for characterizing spatial variations of air pollution within urban areas, identifying emission sources, and enhancing knowledge of atmospheric processes. The Aclima, Inc. mobile measurement and data acquisition platform was used to equip four Google Street View cars with research-grade instruments, two of which were available for the duration of this study. On-road measurements of air quality were made during a series of sampling campaigns between May 2016 and September 2017 at high (i.e., 1-second [s]) temporal and spatial resolution at several California locations: Los Angeles, San Francisco, and the northern San Joaquin Valley (including non-urban roads and the cities of Tracy, Stockton, Manteca, Merced, Modesto, and Turlock). The results demonstrate that the approach is effective for quantifying spatial variations of air pollutant concentrations over measurement periods as short as two weeks. Measurement accuracy and precision are evaluated using results of weekly performance checks and periodic audits conducted through the sampler inlets, which show that research instruments located within stationary vehicles are capable of reliably measuring nitric oxide (NO), nitrogen dioxide (NO), ozone (O), methane (CH) black carbon (BC), and particle number (PN) concentration with bias and precision ranging from <10 % for gases to <25 % for BC and PN at 1-s time resolution. The quality of the mobile measurements in the ambient environment is examined by comparisons with data from an adjacent (< 9 m) stationary regulatory air quality monitoring site and by paired collocated vehicle comparisons, both stationary and driving. The mobile measurements indicate that U.S. EPA classifications of two Los Angeles stationary regulatory monitors' scales of representation are appropriate. Paired time-synchronous mobile measurements are used to characterize the spatial scales of concentration variations when vehicles were separated by <1 to 10 kilometers (km). A data analysis approach is developed to characterize spatial variations while limiting the confounding influence of diurnal variability. The approach is illustrated using data from San Francisco, revealing 1-km scale differences in mean NO and O concentrations up to 117 % and 46 %, respectively, of mean values during a two-week sampling period. In San Francisco and Los Angeles, spatial variations up to factors of 6 to 8 occur at sampling scales of 100 - 300m, corresponding to 1-minute averages.

The United States Environmental Protection Agency (US EPA) list of hazardous air pollutants (HAPs) includes toxic metal suspected or associated with development of cancer. Traditional techniques for detecting and quantifying toxic metals in the atmosphere are either not real time, hindering identification of sources, or limited by instrument costs. Spark emission spectroscopy is a promising and cost-effective technique that can be used for analyzing toxic metals in real time. Here, we have developed a cost-effective spark emission spectroscopy system to quantify the concentration of toxic metals targeted by the US EPA. Specifically, Cr, Cu, Ni, and Pb solutions were diluted and deposited on the ground electrode of the spark emission system. The least absolute shrinkage and selection operator (LASSO) was optimized and employed to detect useful features from the spark-generated plasma emissions. The optimized model was able to detect atomic emission lines along with other features to build a regression model that predicts the concentration of toxic metals from the observed spectra. The limits of detections (LODs) were estimated using the detected features and compared to the traditional single-feature approach. LASSO is capable of detecting highly sensitive features in the input spectrum; however, for some toxic metals the single-feature LOD marginally outperforms LASSO LOD. The combination of low-cost instruments with advanced machine learning techniques for data analysis could pave the path forward for data-driven solutions to costly measurements.

This paper presents the physical basis of the EPIC cloud product algorithms and an initial evaluation of their performance. Since June 2015, EPIC has been providing observations of the sunlit side of the Earth with its 10 spectral channels ranging from the UV to the near-IR. A suite of algorithms has been developed to generate the standard EPIC Level 2 Cloud Products that include cloud mask, cloud effective pressure/height, and cloud optical thickness. The EPIC cloud mask adopts the threshold method and utilizes multichannel observations and ratios as tests. Cloud effective pressure/height is derived with observations from the O A-band (780 nm and 764 nm), and B-band (680 nm and 688 nm) pairs. The EPIC cloud optical thickness retrieval adopts a single channel approach where the 780 nm and 680 nm channels are used for retrievals over ocean and over land, respectively. Comparison with co-located cloud retrievals from geosynchronous earth orbit (GEO) and low earth orbit (LEO) satellites shows that the EPIC cloud product algorithms are performing well and are consistent with theoretical expectations. These products are publicly available at the Atmospheric Science Data Center at the NASA Langley Research Center for climate studies and for generating other geophysical products that require cloud properties as input.

We present an open-path mid-infrared dual-comb spectroscopy (DCS) system capable of precise measurement of the stable water isotopologues HO and HDO. This system ran in a remote configuration at a rural test site for 3.75 months with 60% uptime and achieved a precision of < 2‰ on the normalized ratio of HO and HDO () in 1000s. Here, we compare the values from the DCS system to those from the National Ecological Observatory Network (NEON) isotopologue point sensor network. Over the multi-month campaign, the mean difference between the DCS values and the NEON values from a similar ecosystem is < 2‰ with a standard deviation of 18‰, which demonstrates the inherent accuracy of DCS measurements over a variety of atmospheric conditions. We observe time-varying diurnal profiles and seasonal trends that are mostly correlated between the sites on daily timescales. This observation motivates the development of denser ecological monitoring networks aimed at understanding regional- and synoptic-scale water transport. Precise and accurate open-path measurements using DCS provide new capabilities for such networks.

High-resolution, laboratory, absorption spectra of the oxygen (O) band measured using cavity ring-down spectroscopy were fitted using the Voigt and speed-dependent Voigt line shapes. We found that the speed-dependent Voigt line shape was better able to model the measured absorption coefficients than the Voigt line shape. We used these line shape models to calculate absorption coefficients to retrieve atmospheric total columns abundances of O from ground-based spectra from four Fourier transform spectrometers that are apart of the Total Carbon Column Observing Network (TCCON) Lower O total columns were retrieved with the speed-dependent Voigt line shape, and the difference between the total columns retrieved using the Voigt and speed-dependent Voigt line shapes increased as a function of solar zenith angle. Previous work has shown that carbon dioxide (CO) total columns are better retrieved using a speed-dependent Voigt line shape with line mixing. The column-averaged dry-air mole fraction of CO (XCO) was calculated using the ratio between the columns of CO and O retrieved (from the same spectra) with both line shapes from measurements made over a one-year period at the four sites. The inclusion of speed dependence in the O retrievals significantly reduces the airmass dependence of XCO and the bias between the TCCON measurements and calibrated integrated aircraft profile measurements was reduced from 1% to 0.4%. These results suggest that speed dependence should be included in the forward model when fitting near-infrared CO and O spectra to improve the accuracy of XCO measurements.

Analysis of formaldehyde measurements by the Pandora spectrometer systems between 2016 and 2019 suggested that there was a temperature dependent process inside Pandora head sensor that emitted formaldehyde. Some parts in the head sensor were manufactured from thermal plastic polyoxymethylene homopolimer (E.I. Du Pont de Nemour & Co., USA: POM-H Delrin®) and were responsible for formaldehyde production. Laboratory analysis of the four Pandora head sensors showed that internal formaldehyde production had exponential temperature dependence with a damping coefficient of 0.0911±0.0024 °C and the exponential function amplitude ranging from 0.0041 DU to 0.049 DU. No apparent dependency on the head sensor age and heating/cooling rates was detected. The total amount of formaldehyde internally generated by the POM-H Delrin components and contributing to the direct sun measurements were estimated based on the head sensor temperature and solar zenith angle of the measurements. Measurements in winter, during colder (<10°C) days in general and at high solar zenith angles (> 75 °) were minimally impacted. Measurements during hot days (>28°C) and small solar zenith angles had up to 1 DU (2.69×10 molecules/cm) contribution from POM-H Delrin parts. Multi-axis differential slant column densities were minimally impacted (< 0.01 DU) due to the reference spectrum collected within a short time period with a small difference in head sensor temperature. Three new POM-H Delrin free Pandora head sensors (manufactured in summer 2019) were evaluated for temperature dependent attenuation across the entire spectral range (300 to 530 nm). No formaldehyde or any other absorption above the instrumental noise was observed across the entire spectral range.

Low-cost sensors are often co-located with reference instruments to assess their performance and establish calibration equations, but limited discussion has focused on whether the duration of this calibration period can be optimized. We placed a multipollutant monitor that contained sensors that measure particulate matter smaller than 2.5 μm (PM), carbon monoxide (CO), nitrogen dioxide (NO), ozone (O), and nitric oxide (NO) at a reference field site for one year. We developed calibration equations using randomly selected co-location subsets spanning 1 to 180 consecutive days out of the 1-year period and compared the potential root mean square errors (RMSE) and Pearson correlation coefficients (r). The co-located calibration period required to obtain consistent results varied by sensor type, and several factors increased the co-location duration required for accurate calibration, including the response of a sensor to environmental factors, such as temperature or relative humidity (RH), or cross-sensitivities to other pollutants. Using measurements from Baltimore, MD, where a broad range of environmental conditions may be observed over a given year, we found diminishing improvements in the median RMSE for calibration periods longer than about six weeks for all the sensors. The best performing calibration periods were the ones that contained a range of environmental conditions similar to those encountered during the evaluation period (i.e., all other days of the year not used in the calibration). With optimal, varying conditions it was possible to obtain an accurate calibration in as little as one week for all sensors, suggesting that co-location can be minimized if the period is strategically selected and monitored so that the calibration period is representative of the desired measurement setting.

The inaccurate quantification of personal exposure to air pollution introduces error and bias in health estimations, severely limiting causal inference in epidemiological research worldwide. Rapid advancements in affordable, miniaturised air pollution sensor technologies offer the potential to address this limitation by capturing the high variability of personal exposure during daily life in large-scale studies with unprecedented spatial and temporal resolution. However, concerns remain regarding the suitability of novel sensing technologies for scientific and policy purposes. In this paper we characterise the performance of a portable personal air quality monitor (PAM) that integrates multiple miniaturised sensors for nitrogen oxides (NO ), carbon monoxide (CO), ozone (O) and particulate matter (PM) measurements along with temperature, relative humidity, acceleration, noise and GPS sensors. Overall, the air pollution sensors showed high reproducibility (mean = 0.93, min-max: 0.80-1.00) and excellent agreement with standard instrumentation (mean = 0.82, min-max: 0.54-0.99) in outdoor, indoor and commuting microenvironments across seasons and different geographical settings. An important outcome of this study is that the error of the PAM is significantly smaller than the error introduced when estimating personal exposure based on sparsely distributed outdoor fixed monitoring stations. Hence, novel sensing technologies such as the ones demonstrated here can revolutionise health studies by providing highly resolved reliable exposure metrics at a large scale to investigate the underlying mechanisms of the effects of air pollution on health.

The atmospheric products of the Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm include column water vapor (CWV) at a 1 km resolution, derived from daily overpasses of NASA's Moderate Resolution Imaging Spectroradiometer (MODIS) instruments aboard the Aqua and Terra satellites. We have recently shown that machine learning using extreme gradient boosting (XGBoost) can improve the estimation of MAIAC aerosol optical depth (AOD). Although MAIAC CWV is generally well validated (Pearson's >0.97 versus CWV from AERONET sun photometers), it has not yet been assessed whether machine-learning approaches can further improve CWV. Using a novel spatiotemporal cross-validation approach to avoid overfitting, our XGBoost model, with nine features derived from land use terms, date, and ancillary variables from the MAIAC retrieval, quantifies and can correct a substantial portion of measurement error relative to collocated measurements at AERONET sites (26.9% and 16.5% decrease in root mean square error (RMSE) for Terra and Aqua datasets, respectively) in the Northeastern USA, 2000-2015. We use machine-learning interpretation tools to illustrate complex patterns of measurement error and describe a positive bias in MAIAC Terra CWV worsening in recent summertime conditions. We validate our predictive model on MAIAC CWV estimates at independent stations from the SuomiNet GPS network where our corrections decrease the RMSE by 19.7% and 9.5% for Terra and Aqua MAIAC CWV. Empirically correcting for measurement error with machine-learning algorithms is a postprocessing opportunity to improve satellite-derived CWV data for Earth science and remote sensing applications.