Matt Richardson

From 2016 to 2018 a DC-8 aircraft operated by the US National Aeronautics and Space Administration (NASA) made four series of flights, profiling the atmosphere from 180 m to ∼12 km above sea level (km a.s.l.) from the Arctic to the Antarctic over both the Pacific and Atlantic oceans. This program, the Atmospheric Tomography Mission (ATom), sought to sample the troposphere in a representative manner, making measurements of atmospheric composition in each season. This paper describes the aerosol… Show more

From 2016 to 2018 a DC-8 aircraft operated by the US National Aeronautics and Space Administration (NASA) made four series of flights, profiling the atmosphere from 180 m to ∼12 km above sea level (km a.s.l.) from the Arctic to the Antarctic over both the Pacific and Atlantic oceans. This program, the Atmospheric Tomography Mission (ATom), sought to sample the troposphere in a representative manner, making measurements of atmospheric composition in each season. This paper describes the aerosol microphysical measurements and derived quantities obtained during this mission. Dry size distributions from 2.7 nm to 4.8 µm in diameter were measured in situ at 1 Hz using a battery of instruments: 10 condensation particle counters with different nucleation diameters, two ultra-high-sensitivity aerosol size spectrometers (UHSASs), one of which measured particles surviving heating to 300 ∘C, and a laser aerosol spectrometer (LAS). The dry aerosol measurements were complemented by size distribution measurements from 0.5 to 930 µm diameter at near-ambient conditions using a cloud, aerosol, and precipitation spectrometer (CAPS) mounted under the wing of the DC-8. Dry aerosol number, surface area, and volume, and optical scattering and asymmetry parameters at several wavelengths from the near-UV to the near-IR ranges were calculated from the measured dry size distributions (2.7 nm to 4.8 µm). Dry aerosol mass was estimated by combining the size distribution data with particle density estimated from independent measurements of aerosol composition with a high-resolution aerosol mass spectrometer and a single-particle soot photometer. We describe the instrumentation and fully document the aircraft inlet and flow distribution system, the derivation of uncertainties, and the calculation of data products from combined size distributions.... Show less

Atmospheric aerosol is a key component of the chemistry and climate of the Earth's atmosphere. Accurate measurement of the concentration of atmospheric particles as a function of their size is fundamental to investigations of particle microphysics, optical characteristics, and chemical processes. We describe the modification, calibration, and performance of two commercially available, Ultra-High Sensitivity Aerosol Spectrometers (UHSASs) as used on the NASA DC-8 aircraft during the Atmospheric… Show more

Atmospheric aerosol is a key component of the chemistry and climate of the Earth's atmosphere. Accurate measurement of the concentration of atmospheric particles as a function of their size is fundamental to investigations of particle microphysics, optical characteristics, and chemical processes. We describe the modification, calibration, and performance of two commercially available, Ultra-High Sensitivity Aerosol Spectrometers (UHSASs) as used on the NASA DC-8 aircraft during the Atmospheric Tomography Mission (ATom). To avoid sample flow issues related to pressure variations during aircraft altitude changes, we installed a laminar flow meter on each instrument to measure sample flow directly at the inlet as well as flow controllers to maintain constant volumetric sheath flows. In addition, we added a compact thermodenuder operating at 300 ∘C to the inlet line of one of the instruments. With these modifications, the instruments are capable of making accurate (ranging from 7 % for Dp < 0.07 µm to 1 % for Dp > 0.13 µm), precise (< ±1.2 %), and continuous (1 Hz) measurements of size-resolved particle number concentration over the diameter range of 0.063–1.0 µm at ambient pressures of > 1000 to 225 hPa, while simultaneously providing information on particle volatility.

We assessed the effect of uncertainty in the refractive index (n)... Show less

Natural emissions of ozone-and-aerosol-precursor gases such as isoprene and monoterpenes are high in the southeastern US. In addition, anthropogenic emissions are significant in the southeastern US and summertime photochemistry is rapid. The NOAA-led SENEX (Southeast Nexus) aircraft campaign was one of the major components of the Southeast Atmosphere Study (SAS) and was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants. During SENEX… Show more

Natural emissions of ozone-and-aerosol-precursor gases such as isoprene and monoterpenes are high in the southeastern US. In addition, anthropogenic emissions are significant in the southeastern US and summertime photochemistry is rapid. The NOAA-led SENEX (Southeast Nexus) aircraft campaign was one of the major components of the Southeast Atmosphere Study (SAS) and was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants. During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN.

Here we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign. The aircraft, its capabilities and standard measurements are described. The instrument payload is summarized including detection limits, accuracy, precision and time resolutions for all gas-and-aerosol phase instruments. The inter-comparisons of compounds measured with multiple instruments on the NOAA WP-3D are presented and were all within the stated uncertainties, except two of the three NO2 measurements.

The SENEX flights included day- and nighttime flights in the southeastern US as well as flights over areas with intense shale gas extraction (Marcellus, Fayetteville and Haynesville shale). We present one example flight on 16 June 2013, which was a daytime flight over the Atlanta region, where several crosswind transects of plumes from the city and nearby point sources, such as power plants, paper mills and landfills, were flown. The area around Atlanta has large biogenic isoprene emissions, which provided an excellent case for studying the interactions between biogenic and anthropogenic emissions. In this example flight, chemistry in and outside the Atlanta plumes was observed for several hours after emission. The analysis of this flight showcases the strategies implemented to answer some of the main SENEX science questions. Show less

Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US). Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0–4 km aggregate profiles and a simple… Show more

Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US). Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0–4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD) to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH). For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry–climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of  ∼  25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1–0.5 µm diameter dominates aerosol extinction. Show less

A light-weight, low-cost optical particle spectrometer for measurements of aerosol number concentrations and size distributions has been designed, constructed, and demonstrated. The spectrometer is suitable for use on small, unmanned aerial vehicles (UAVs) and in balloon sondes. The spectrometer uses a 405 nm diode laser to count and size individual particles in the size range 140–3000 nm. A compact data system combines custom electronics with a single-board commercial computer. Power… Show more

A light-weight, low-cost optical particle spectrometer for measurements of aerosol number concentrations and size distributions has been designed, constructed, and demonstrated. The spectrometer is suitable for use on small, unmanned aerial vehicles (UAVs) and in balloon sondes. The spectrometer uses a 405 nm diode laser to count and size individual particles in the size range 140–3000 nm. A compact data system combines custom electronics with a single-board commercial computer. Power consumption is 7W at 9–15 V. 3D printing technology was used in the construction of the instrument to reduce cost, manufacturing complexity, and weight. The resulting Printed Optical Particle Spectrometer (POPS) instrument weighs about 800 g with an approximate materials cost of 2500 USD. Several POPS units have been constructed, tested in the laboratory, and deployed on UAVs. Here we present an overview of the instrument design and construction, laboratory validation data, and field engineering data for POPS. Show less

Laboratory experiments were conducted to assess the suitability of photoacoustic spectroscopy (PAS) for aerosol absorption measurement at high relative humidity (RH). Initial experiments characterized the PAS sensitivity that increased strongly by ∼1.25 between dry conditions and 90% RH. Correction procedures were validated by measuring RH-independent absorption for hydrophobic absorbing particles. Absorption measured by PAS for a range of hygroscopic particles, including different… Show more

Laboratory experiments were conducted to assess the suitability of photoacoustic spectroscopy (PAS) for aerosol absorption measurement at high relative humidity (RH). Initial experiments characterized the PAS sensitivity that increased strongly by ∼1.25 between dry conditions and 90% RH. Correction procedures were validated by measuring RH-independent absorption for hydrophobic absorbing particles. Absorption measured by PAS for a range of hygroscopic particles, including different morphologies, hygroscopicities, and absorbing entities, showed strong low biases at high RH (down to 0.4 at 90% RH). The bias was due to water evaporation impacting the PAS signal. Cooling samples to lower absolute humidity while maintaining a constant RH did not significantly reduce the bias magnitude within the temperature range 11–25°C. The magnitude and RH dependence of the bias were not reproduced well using a model of PAS response incorporating coupled heat and mass transfer in the transition regime. This was attributed, in part, to uncertainty related to changes in the water mass accommodation coefficient with RH. Given our inability to correct for evaporation-induced bias effects accurately, or reduce their magnitude experimentally, we conclude that PAS is not a technique well suited to the measurement of absorption at high RH. In order to minimize RH-related errors in PAS measurements made under notionally “dry” conditions, we recommend operation in the RH range 10–30%. Show less

This paper describes the design and performance of a photo-acoustic aerosol absorption spectrometer (PAS) built for operation on a research aircraft platform. The PAS instrument is capable of measuring dry absorption at 659 nm, 532 nm, and 404 nm, and absorption enhancement due to coatings at 532 nm and 404 nm. The measurement accuracy for all channels is < = 10% and in flight 1 Hz sensitivities lie within the range of 0.5–1.5 Mm−1. PAS measurements of calibrated absorbing aerosol samples… Show more

This paper describes the design and performance of a photo-acoustic aerosol absorption spectrometer (PAS) built for operation on a research aircraft platform. The PAS instrument is capable of measuring dry absorption at 659 nm, 532 nm, and 404 nm, and absorption enhancement due to coatings at 532 nm and 404 nm. The measurement accuracy for all channels is < = 10% and in flight 1 Hz sensitivities lie within the range of 0.5–1.5 Mm−1. PAS measurements of calibrated absorbing aerosol samples are shown to be consistent with measurements made by a previous generation single channel photo-acoustic instrument. Aircraft data collected during a recent field campaign in California are used to demonstrate the capabilities of the PAS. In combination with an aircraft cavity ring down aerosol extinction spectrometer described in a companion paper, the new PAS instrument provides a sensitive airborne in-situ characterization of aerosol optics. Show less

High quality in situ observations of aerosol particle optical properties, namely extinction, scattering and absorption, provide important information needed to constrain the role of aerosols in the climate system. This paper outlines the design and performance of an aircraft instrument utilising cavity ringdown spectroscopy for the measurement of aerosol extinction. The 8‑channel cavity ringdown spectrometer measures extinction at multiple wavelengths (405, 532 and 662 nm) and at multiple… Show more

High quality in situ observations of aerosol particle optical properties, namely extinction, scattering and absorption, provide important information needed to constrain the role of aerosols in the climate system. This paper outlines the design and performance of an aircraft instrument utilising cavity ringdown spectroscopy for the measurement of aerosol extinction. The 8‑channel cavity ringdown spectrometer measures extinction at multiple wavelengths (405, 532 and 662 nm) and at multiple relative humidities (e.g. 10 %, 70 %, 95 %). Key performance characteristics include a 1 s detection limit better than 0.1 Mm, accuracy of < 2 % for dry aerosol measurements and a 1 s precision better than 40 % for extinction levels > 10 Mm. Laboratory and field data demonstrate that the 1 s precision is limited by the statistics of aerosol particles in the laser beam rather than the precision of the extinction measurement per se. The measurement precision improves with averaging to 5 % at 60 s for extinction levels > 10 Mm. Field data collected during a recent airborne campaign in California, which involved 18 research flights during May and June 2010, are used to demonstrate the in-flight performance of the new instrument. Show less

Knowledge of cloud and precipitation formation processes remains incomplete, yet global precipitation is predominantly produced by clouds containing the ice phase. Ice first forms in clouds warmer than -36 °C on particles termed ice nuclei. We combine observations from field studies over a 14-year period, from a variety of locations around the globe, to show that the concentrations of ice nuclei active in mixed-phase cloud conditions can be related to temperature and the number concentrations… Show more

Knowledge of cloud and precipitation formation processes remains incomplete, yet global precipitation is predominantly produced by clouds containing the ice phase. Ice first forms in clouds warmer than -36 °C on particles termed ice nuclei. We combine observations from field studies over a 14-year period, from a variety of locations around the globe, to show that the concentrations of ice nuclei active in mixed-phase cloud conditions can be related to temperature and the number concentrations of particles larger than 0.5 μm in diameter. This new relationship reduces unexplained variability in ice nuclei concentrations at a given temperature from ∼103 to less than a factor of 10, with the remaining variability apparently due to variations in aerosol chemical composition or other factors. When implemented in a global climate model, the new parameterization strongly alters cloud liquid and ice water distributions compared to the simple, temperature-only parameterizations currently widely used. The revised treatment indicates a global net cloud radiative forcing increase of ∼1 W m-2 for each order of magnitude increase in ice nuclei concentrations, demonstrating the strong sensitivity of climate simulations to assumptions regarding the initiation of cloud glaciation. Show less

The mass accommodation coefficient for uptake of water vapor to liquid water, αM, has been constrained using photoacoustic measurements of aqueous absorbing aerosol. Measurements performed over a range of relative humidities and pressures were compared to detailed model calculations treating coupled heat and mass transfer occurring during photoacoustic laser heating cycles. The strengths and weaknesses of this technique are very different to those for droplet growth/evaporation experiments that… Show more

The mass accommodation coefficient for uptake of water vapor to liquid water, αM, has been constrained using photoacoustic measurements of aqueous absorbing aerosol. Measurements performed over a range of relative humidities and pressures were compared to detailed model calculations treating coupled heat and mass transfer occurring during photoacoustic laser heating cycles. The strengths and weaknesses of this technique are very different to those for droplet growth/evaporation experiments that have typically been applied to these measurements, making this a useful complement to existing studies. Our measurements provide robust evidence that αM is greater than 0.1 for all humidities tested and greater than 0.3 for data obtained at relative humidities greater than 88% where the aerosol surface was most like pure water. These values of αM are above the threshold at which kinetic limitations are expected to impact the activation and growth of aerosol particles in warm cloud formation. Show less