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Remote Measurement of Pollution - A 40-Year Langley Retrospective: Temperature and Gaseous Species - Part 1

The National Aeronautics and Space Administration (NASA) phased down its Apollo Moon Program after 1970 in favor of a partly reusable Space Shuttle vehicle that could be used to construct and supply a manned, Earth-orbiting Space Station. Applications programs were emphasized in response to the growing public concern about Earth's finite natural resources and the degradation of its environment. Shortly thereafter, a workshop was convened in Norfolk, Virginia, on Remote Measurement of Pollution (or RMOP), and its findings are in a NASA Special Publication (NASA SP-285). The three primary workshop panels and their chairmen were focused on trace gas species (Will Kellogg), atmospheric particulates or aerosols (Verner Suomi), and water pollution (Gifford Ewing). Many of the workshop participants were specialists in the techniques that might be employed for the regional to global-scale, remote measurements from an Earth-orbiting satellite. The findings and recommendations of the RMOP Report represent the genesis of and a blueprint for the satellite, atmospheric sensing programs within NASA for nearly two decades. This paper is a brief, 40-year retrospective of those instrument developments that were an outgrowth of the RMOP activity. Its focus is on satellite measurement capabilities for temperature and gaseous species that were demonstrated by atmospheric technologists at the Langley Research Center. Limb absorption by solar occultation, limb infrared radiometry, and gas filter correlation radiometry techniques provided significant science data, so they are emphasized in this review.

Remsberg, Ellis E.↗

Laser Heterodyne Radiometer for Sensitive Detection of CO2 and CH4

We propose to develop an inexpensive, miniaturized, passive laser heterodyne radiometer (LHR) using commercially available telecommunications laser components to measure two significant carbon cycle gases in the atmospheric column: carbon dioxide (CO2) and methane (CH4). This instrument would operate in tandem with the passive aerosol sensor currently used in AERONET (an established network of more than 450 ground aerosol monitoring instruments worldwide). Because aerosols induce a radiative effect that influences terrestrial carbon exchange, simultaneous detection of aerosols with these key carbon cycle gases offers a uniquely comprehensive measurement approach that supports the Decadal Survey. Laser heterodyne radiometry is a technique for detecting weak signals that was adapted from radio receiver technology. In a radio receiver, a weak input signal from a radio antenna is mixed with a stronger local oscillator signal. The mixed signal (beat note, or intermediate frequency) has a frequency equal to the difference between the input signal and the local oscillator. The intermediate frequency is amplified and sent to a detector that extracts the audio from the signal. In a laser heterodyne radiometer, the weak input signal is light that has undergone absorption by a trace gas. The local oscillator is a laser at a near-by frequency - in this case a low-cost distributed feedback (DFB) telecommunications laser. These two light waves are superimposed in either a beamsplitter or in a fiber coupler (as is the case in this design). The signals are mixed in the detector, and the RF beat frequency is extracted. Changes in concentration of the trace gas are realized through analyzing changes in the beat frequency amplitude. A schematic of the progression of the LHR development project is shown in the figure below. At the center (within the dashed line), light from the local oscillator is superimposed upon light that has undergone absorption by a trace gas, in a single mode fiber coupler. Superimposed light is mixed in a fast photoreceiver, and the beat signal is analyzed for changes in absorption. The left portion of the figure depicts a progression of light sources that pass through the trace gas, increasing in complexity in the downward direction. On the right side of the figure, RF signal processing progresses from a commercially available spectrum analyzer to a RF receiver, and finally to an RF filter bank to deconvolute portions of the beat frequency more heavily weighted for different altitudes.

Wilson, Emily L.↗

Effect of tropospheric aerosols upon atmospheric infrared cooling rates

An investigation has been made of the impact of wind-blown dust particles upon local climate of arid regions. The case of Northwest India is specifically considered, where a dense layer of dust persists for several months during the summer. In order to examine the effect of this dust layer on the infrared radiative flux and cooling rates, a method is presented for calculating the IR flux within a dusty atmosphere which allows the use of gaseous band models and is applicable in the limit of small single scattering albedo and pronounced forward scattering. The participating components of the atmosphere are assumed to be water vapor and spherical quartz particles only. The atmospheric window is partially filled by including the water vapor continuum bands for which empirically obtained transmission functions have been used. It is shown that radically different conclusions may be drawn on dust effects if the continuum absorption is not considered. The radiative transfer model, when applied to a dusty atmosphere, indicates that there is a moderate enhancement in the atmospheric greenhouse and a 10% increase in the mean IR radiative cooling rate, relative to the dust free case, within the lower troposphere. These results have been compared with previous work by other authors in the context of the possibility of dust layers inhibiting local precipitation.

Harshvardhan, MR.↗

North Slope of Alaska Black Carbon Loadings and Mixing State for MOSAiC Field Campaign Report

The Arctic represents a unique region to study global climate change in that it exhibits pronounced sensitivity towards aerosol radiative forcing, referred to as arctic amplification. Of the aerosol species that are expected to contribute to this aerosol forcing, black carbon (BC) is arguably at the top of the list. Black carbon has this distinction because it exerts two radiative forcing influences that can be characterized as atmospheric and non-atmospheric. As an atmospheric forcer, BC behaves much as it does in the mid-latitudes – through the direct effect and semi-direct effects – collectively causing surface dimming with subsequent surface cooling and mid-altitude warming affecting cloud cover. As a terrestrial forcer, which is unique to the cryosphere, the deposition of BC on the surface can readily decrease polar surface albedo that, in turn, can activate a positive feedback wherein the increased surface absorption leads to further snow melt causing still further reduction in surface albedo.

54 ENVIRONMENTAL SCIENCES↗

Development of a Portable, Ground-Based Ozone Lidar Instrument for Tropospheric Ozone Research and Educational Training

The objective of this project is to develop a portable, eye-safe, ground-based ozone lidar instrument specialized for ozone differential absorption lidar (DIAL) measurements in the troposphere. This prototype instrument is intended to operate at remote field sites and to serve as the basic unit for monitoring projects requiring multi-instrument networks, such as that discussed in the science plan for the Global Tropospheric Ozone Project (GTOP). This instrument will be based at HU for student training in lidar technology as well as atmospheric ozone data analysis and interpretation. It will be also available for off-site measurement campaigns and will serve as a test bed for further instrument development. Later development beyond this grant to extend the scientific usefulness of the instrument may include incorporation of an aerosol channel and upgrading the laser to make stratospheric ozone measurements. Undergraduate and graduate students have been and will be active participants in this research effort.

Chyba, Thomas↗

Aeolus -A Mission to Study the Thermal and Wind Environment of Mars

Aeolus is a small satellite mission to observe surface and atmospheric forcing and general circulation of Mars, by measuring surface energy balance, atmospheric temperatures, aerosols and clouds, and winds. Critically, Aeolus will make these measurements at all local times of day, providing information on both seasonal and diurnal variability. To date, direct measurements of Martian wind speeds have only been possible at the surface, only during daylight hours, and over small areas limited by rover traverse capabilities. From orbit, thermal measurements (e.g., estimates from assumed geostrophic balance) as well as images of dust storms and dune migration have provided inputs to derive current data sets on Martian winds. However, Mars General Circulation models demonstrate that wind speeds derived from these indirect measurements may be in error by 50 to 100%. For this reason, direct wind velocity measurements have been deemed "High Priority" by MEPAG (Mars Exploration Program Analysis Group); measuring wind speeds and corresponding thermal data is vital to understanding the climate of Mars. Aeolus will carry four Spatial Heterodyne Spectrometers (SHS), coupled to two orthogonal viewing telescopes. These high-resolution near-infrared spectrometers will measure CO2 (daytime absorption) and O2 (day and night emission) lines in the Martian atmosphere. Doppler shifts in these lines can be measured during Martian day and night, resolving wind speeds down to ~5 m/s. Orthogonal views allow the spectrometers to capture wind vectors over all observation locations. Aeolus will also carry the atmospheric limb-viewing Thermal Limb Sounder (TLS) to measure atmospheric temperatures, water ice clouds, and dust abundances across all altitudes where winds are measured. Finally, the Surface Radiometric Sensor Package (SuRSeP), a nadir viewing radiometer, will measure the total reflected solar and emitted thermal radiance, surface temperature, and water cloud and dust total column abundances. The combined spectral and thermal measurements will provide a new understanding of the global energy balance, dust transport processes, and climate cycles in the Martian atmosphere. Aeolus will consist of a single satellite in a near-polar orbit, allowing it to pass over all local times, with the baseline mission observing all seasons of an entire Martian year (two Earth years). Aeolus was one of two Martian smallsat concepts selected for study through the Planetary Science Deep Space SmallSat Studies program. This talk will provide an overview of the mission, including science rationale, instruments, spacecraft, and mission operations concept.

and winds↗

Particle phase-state variability in the North Atlantic free troposphere during summertime is determined by atmospheric transport patterns and sources

Abstract. Free tropospheric aerosol particles have important but poorly constrained climate effects due to transformations of their physicochemical properties during long-range transport. In this study, we investigate the chemical composition and provide an overview of the phase states of individual particles that have undergone long-range transport over the North Atlantic Ocean in June and July 2014, 2015, and 2017 to the Observatory of Mount Pico (OMP) in the Azores. The OMP is an ideal site for studying long-range-transported free tropospheric particles because local emissions have a negligible influence and contributions from the boundary layer are rare. We used the FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) to determine the origins and transport trajectories of sampled air masses and found that most of them originated from North America and recirculated over the North Atlantic Ocean. The FLEXPART analysis showed that the sampled air masses were highly aged (average plume age >10 d). Size-resolved chemical compositions of individual particles were probed using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). CCSEM-EDX results showed that the most abundant particle types were carbonaceous (∼ 29.9 % to 82.0 %), sea salt (∼ 0.3 % to 31.6 %), and sea salt with sulfate (∼ 2.4 % to 31.5 %). We used a tilted stage interfaced within an environmental scanning electron microscope (ESEM) to determine the phase states of individual submicron particles. We found that most particles (∼ 47 % to 99 %) were in the liquid state at the time of collection due to inorganic inclusions. Moreover, we also observed substantial fractions of solid and semisolid particles (∼ 0 % to 30 % and ∼ 1 % to 42 %, respectively) during different transport patterns and events, reflecting the particles' phase-state variability for different atmospheric transport events and sources. Combining phase state measurements with FLEXPART CO tracer analysis, we found that wildfire-influenced plumes can result in particles with a wide range of viscosities after long-range transport in the free troposphere. We also used temperature and RH values extracted from the Global Forecast System (GFS) along the FLEXPART-simulated path to predict the phase state of the particles during transport and found that neglecting internal mixing with inorganics would lead to an overestimation of the viscosity of free tropospheric particles. Our findings warrant future investigation aiming at the quantitative assessment of the influence of internal mixing on the phase states of the individual particles. This study also provides insights into the chemical composition and phase state of free tropospheric particles, which can help models to reduce uncertainties about the effects of ambient aerosol particles on climate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The atmosphere of Jupiter - An analysis of the Voyager radio occultation measurements

Coherently related S and X band signals of 2.3 and 8.4 GHz, respectively, which were transmitted from Voyagers 1 and 2 were used to probe the Jovian atmosphere. Height profiles of the gas refractivity, molecular number density, pressure, temperature, and microwave absorption in the troposphere and stratosphere were observed at latitudes ranging from 0 to 70 deg S. At 1000 mbar, the temperature was + or - 5 K and the lapse rate was equal to the adiabatic value of 2.1 K/km within the resolution of the measurements. The ammonia abundance in this region was 0.022 + or - 0.008%, which is in good agreement with values derived from cosmic abundance considerations. The tropopause at the 140 mbar level had a temperature of 110 K, which increased with increasing altitude, reaching 160 + or - 20 K in the 10 to 1 mbar region. Significant horizontal density variations were detected in the stratosphere, which implies a nonuniform temperature and aerosol distribution across the Jovian disk or across high- and low-pressure regions due to local atmospheric dynamics.

Lindal, G. F.↗

Precipitable water vapor over oceans from the Maritime Aerosol Network: Evaluation of global models and satellite products under clear sky conditions

We present results from an evaluation of precipitable water vapor (W) over remote oceanic areas as derived from global reanalysis models and from satellites against observations from the Maritime Aerosol Network (MAN) for cloudless skies during the period of 2004–2017. They cover polar, mid latitude and tropical oceanic regions and represent a first effort to use MAN observations for such evaluation. The global reanalysis model products evaluated in this study are from the Modern-Era Retrospective analysis for Research and Applications Version 2 (MERRA-2), the European Centre for Medium-Range Weather Forecasts (ECMWF) Interim Reanalysis (ERA I), and the Climate Forecast System Reanalysis (CFSR) model. The satellite products evaluated are from the Moderate Resolution Imaging Spectroradiometer (MODIS), the Polarization and Directionality of the Earth's Reflectances (POLDER), the Global Ozone Monitoring Experiment (GOME-2), the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY), and the Atmospheric Infra-red Sounder (AIRS). Satellite retrievals of W are based on the attenuation of solar reflected light by water vapor absorption bands, except those from AIRS that rely on brightness temperature measurements. A very good agreement is observed between the model estimates and MAN, with mean differences of ~5% and standard deviations of ~15%. These results are within the uncertainties associated with the models and the measurements, indicating the skill of the reanalysis models to estimate W over oceans under clear sky conditions. Mean differences of W between the satellite and MAN products are ~11, 6.7, 12, −7, and 3% for MODIS, POLDER, GOME-2, SCIAMACHY and AIRS respectively, while their standard deviations are 31, 29, 28, 20 and 17%. These differences reveal the need to address inconsistencies among different satellite sensors and ground-based measurements to reduce the uncertainties associated with the retrievals.

Daniel Pérez-Ramírez↗

A Superposition Technique for Deriving Photon Scattering Statistics in Plane-Parallel Cloudy Atmospheres

Photon transport in a multiple scattering medium is critically dependent on scattering statistics, in particular the average number of scatterings. A superposition technique is derived to accurately determine the average number of scatterings encountered by reflected and transmitted photons within arbitrary layers in plane-parallel, vertically inhomogeneous clouds. As expected, the resulting scattering number profiles are highly dependent on cloud particle absorption and solar/viewing geometry. The technique uses efficient adding and doubling radiative transfer procedures, avoiding traditional time-intensive Monte Carlo methods. Derived superposition formulae are applied to a variety of geometries and cloud models, and selected results are compared with Monte Carlo calculations. Cloud remote sensing techniques that use solar reflectance or transmittance measurements generally assume a homogeneous plane-parallel cloud structure. The scales over which this assumption is relevant, in both the vertical and horizontal, can be obtained from the superposition calculations. Though the emphasis is on photon transport in clouds, the derived technique is applicable to any scattering plane-parallel radiative transfer problem, including arbitrary combinations of cloud, aerosol, and gas layers in the atmosphere.

Platnick, S.↗

Clear-Sky Surface Solar Radiation During South China Sea Monsoon Experiment

Downward solar fluxes measured at Dungsha coral island (20 deg. 42 min. N, 116 deg. 43 min. E) during the South China Sea Monsoon Experiment (May-June 1998) have been calibrated and compared with radiative transfer calculations for three clear-sky days. Model calculations use water vapor and temperature profiles from radiosound measurements and the aerosol optical thickness derived from sunphotometric radiance measurements at the surface. Results show that the difference between observed and model-calculated downward fluxes is less than 3% of the daily mean. Averaged over the three clear days, the difference reduces to 1%. The downward surface solar flux averaged over the three days is 314 W per square meters from observations and 317 W per square meters from model calculations, This result is consistent with a previous study using TOGA CAORE measurements, which found good agreements between observations and model calculations. This study provides an extra piece of useful information on the modeling of radiative transfer, which fills in the puzzle of the absorption of solar radiation in the atmosphere.

Lin, Po-Hsiung↗

Polarimetric Retrievals of Cloud Droplet Number Concentrations

Cloud droplet number concentration (Nd) is an important parameter of liquid clouds and is crucial to understanding aerosol-cloud interactions. It couples boundary layer aerosol composition, size and concentration with cloud reflectivity. It affects cloud evolution, precipitation, radiative forcing, global climate and, through observation, can be used to partially monitor the first indirect effect. With its unique combination of multi-wavelength, multi-angle, total and polarized reflectance measurements, the Research Scanning Polarimeter (RSP) retrieves Nd with relatively few assumptions. The approach involves measuring cloud optical thickness, mean droplet extinction cross-section and cloud physical thickness. Polarimetric observations are capable of measuring the effective variance, or width, of the droplet size distribution. Estimating cloud geometrical thickness is also an important component of the polarimetric Nd retrieval, which is accomplished using polarimetric measurements in a water vapor absorption band to retrieve the amount of in-cloud water vapor and relating this to physical thickness. We highlight the unique abilities and quantify uncertainties of the polarimetric approach. We validate the approach using observational data from the North Atlantic and Marine Ecosystems Study (NAAMES). NAAMES targets specific phases in the seasonal phytoplankton lifecycle and ocean-atmosphere linkages. This study provides an excellent opportunity for the RSP to evaluate its approach of sensing Nd over a range of concentrations and cloud types with in situ measurements from a Cloud Droplet Probe (CDP). The RSP and CDP, along with an array of other instruments, are flown on the NASA C-130 aircraft, which flies in situ and remote sensing legs in sequence. Cloud base heights retrieved by the RSP compare well with those derived in situ (R=0.83) and by a ceilometer aboard the R.V. Atlantis (R=0.79). Comparing geometric mean values from 12 science flights throughout the NAAMES-1 and NAAMES-2 campaigns, we find a strong correlation between Nd retrieved by the RSP and CDP (R=0.96). A linear least squares fit has a slope of 0.92 and an intercept of 0.3 cm−3. Uncertainty in this comparison can be attributed to cloud 3D effects, nonlinear liquid water profiles, multilayered clouds, measurement uncertainty, variation in spatial and temporal sampling, and assumptions used within the method. Radiometric uncertainties of the RSP measurements lead to biases on derived optical thickness and cloud physical thickness, but these biases largely cancel out when deriving Nd for most conditions and geometries. We find that a polarimetric approach to sensing Nd is viable and the RSP is capable of accurately retrieving Nd for a variety of cloud types and meteorological conditions.

Droplet concentration↗

DIAL Measurements of Free-Tropospheric Ozone Profiles in Huntsville, AL

A tropospheric ozone Differential Absorption Lidar (DIAL) system, developed jointly by NASA and the University of Alabama at Huntsville (UAH), measures free-tropospheric ozone profiles between 4-10 km. Located at 192 meters altitude in the Regional Atmospheric Profiling Laboratory for Discovery (RAPCD) on the UAH campus in Huntsville, AL, USA, this tropospheric ozone lidar operates under both daytime and nighttime conditions. Frequent coincident ozonesonde flights and theoretical calculations provide evidence to indicate the retrieval accuracy ranges from better than 8% at 4km to 40%-60% at 10 kin with 750-m vertical resolution and 30-minute integration. With anticipated improvements to allow retrievals at both higher and lower altitudes, this ozone lidar, along with co-located aerosol and Doppler Wind Lidars, will provide a unique 18 dataset for investigations of PBL and free-tropospheric chemical and dynamic processes.

Kuang, Shi↗

Chemistry and dynamics of the lower troposphere over North America and the North Atlantic Ocean in fall 1997 observed using an airborne UV DIAL system

The NASA Langley Research Center's airborne UV Differential Absorption Lidar (DIAL) system participated in the Subsonic Assessment, Ozone and Nitrogen Oxide Experiment (SONEX) mission from October 13 to November 12, 1997. The purpose of the mission was to study the upper troposphere/lower stratosphere in and near the North Atlantic flight corridor to better understand this region of the atmosphere and how civilian air travel in the corridor might be affecting the atmospheric chemistry. Bases of operations included NASA Ames, California (37.4 deg N, 122.1 deg W); Bangor, Maine (44.8 deg N, 68.8 deg W); Shannon, Ireland (52.7 deg N, 8.9 deg W); and Lajes, Terceira Island, Azores (38.8 deg N, 27.1 deg W). Since the UV DIAL system observes in the nadir as well as the zenith, aerosol and ozone data were obtained from near the Earth's surface to the lower stratosphere. A number of interesting features were noted relating to both chemistry and dynamics of the troposphere, which are reported here.

Grant, William B.↗

Net Radiative Effects of Dust in the Tropical North Atlantic Based on Integrated Satellite Observations and in Situ Measurements

In this study, we integrate recent in situ measurements with satellite retrievals of dust physical and radiative properties to quantify dust direct radiative effects on shortwave (SW) and longwave (LW) radiation (denoted as DRESW and DRELW, respectively) in the tropical North Atlantic during the summer months from 2007 to 2010. Through linear regression of the CERES-measured top-of atmosphere (TOA) flux versus satellite aerosol optical depth (AOD) retrievals, we estimate the instantaneous DRESW efficiency at the TOA to be -49+/-7.1 W/sq.m AOD(exp -1) and -36+/-4:8W/sq.m AOD(exp -1) based on AOD from MODIS and CALIOP, respectively. We then perform various sensitivity studies based on recent measurements of dust particle size distribution (PSD), refractive index, and particle shape distribution to determine how the dust microphysical and optical properties affect DRE estimates and its agreement with the above-mentioned satellite-derived DREs. Our analysis shows that a good agreement with the observation-based estimates of instantaneous DRESW and DRELW can be achieved through a combination of recently observed PSD with substantial presence of coarse particles, a less absorptive SW refractive index, and spheroid shapes. Based on this optimal combination of dust physical properties we further estimate the diurnal mean dust DRE(sub SW) in the region of -10W/sq.m at TOA and -26W/sq.m at the surface, respectively, of which ~30% is canceled out by the positive DRE(sub LW). This yields a net DRE of about -6:9 and -18.3 W/sq.m at TOA and the surface, respectively. Our study suggests that the LW flux contains useful information on dust particle size, which could be used together with SW observations to achieve a more holistic understanding of the dust radiative effect.

Song, Qianqian↗

Development and characterization of an aerosol-generated multi-method analytical particle test material

Ceria (CeO 2 ) particles with low to ultra-low loading of nickel dopant were produced using an aerosol-based, droplet-to-particle synthesis via an in-line calcination technique. This aerosol-based synthesis method enables the production of particles with a monodisperse size distribution. These produced and well-characterized, multi-element, ceria-based particles demonstrate a material exemplar for multi-method analytical testing. They were prepared from a cerium nitrate feedstock where low loading nickel dopant was added at target Ni/(Ni + Ce) atomic percents of 1 %, 0.1 %, and 0.01 %, using a nickel nitrate spike. This methodology proved to produce ceria particles doped with a dynamic range of low to ultra-low loadings of nickel over a 24-h period, with consistent size distribution, morphology, and composition. The successful incorporation of nickel was demonstrated with bulk and single particle inductively coupled plasma mass spectroscopy and revealed notable particle-to-particle elemental homogeneity. X-ray photoelectron spectroscopy demonstrated the presence of a high concentration of nickel dopant incorporated preferentially toward the surface of the particles, and that this dopant aided oxidation of surface Ce(III) atoms to Ce(IV). These particle test materials were then validated through X-ray absorption near edge spectroscopy, comparing the ultra-low 0.01 % Ni and low 1 % Ni-doped ceria samples. This revealed a more-reduced oxidation state of the nickel with an increase in dopant concentration. Finally, this work demonstrates a synthesis and systematic characterization scheme to produce multi-method analytical test particulates.

36 MATERIALS SCIENCE↗

Modeling Functional Organic Chemistry in Arctic Rivers: An Idealized Siberian System

Rivers of the Arctic will become ever more important for the global climate, since they carry a majority of continental dissolved organic carbon flux into the rapidly changing polar ocean. Aqueous organics comprise a wide array of functional groups, several of which are likely to impact coastal and open water biophysical properties. Light attenuation, interfacial films, aerosol formation, gas release and momentum exchange can all be cited. We performed Lagrangian kinetic modeling for the evolution of riverine organic chemistry as the molecules in question make their way from the highlands to Arctic outlets. Classes as diverse as the proteins, sugars, lipids, re-condensates, humics, bio-tracers and small volatiles are all included. Our reduced framework constitutes an idealized northward flow driving a major hydrological discharge rate and primarily representing the Russian Lena. Mountainous, high solute and tundra sources are all simulated, and they meet up at several points between soil and delta process reactors. Turnover rates are parameterized beginning with extrapolated coastal values imposed along a limited tributary network, with connections between different terrestrial sub-ecologies. Temporal variation of our total dissolved matter most closely resembles the observations when we focus on the restricted removal and low initial carbon loads, suggesting relatively slow transformation along the water course. Thus, channel combinations and mixing must play a dominant role. Nevertheless, microbial and photochemical losses help determine the final concentrations for most species. Chemical evolution is distinct for the various functionalities, with special contributions from pre- and post-reactivity in soil and delta waters. Several functions are combined linearly to represent the collective chromophoric dissolved matter, characterized here by its absorption. Tributaries carry the signature of lignin phenols to segregate tundra versus taiga sources, and special attention is paid to the early then marine behaviors of low molecular weight volatiles. Heteropolycondensates comprise the largest percentage of reactive carbon in our simulations due to recombination/accumulation, and they tend to be preeminent at the mouth. Outlet concentrations of individual structures such as amino acids and absorbers lie above threshold values for biophysical influence, on the monolayer and light attenuation. The extent of coastal spreading is examined through targeted regional box modeling, relying on salinity and color for calibration. In some cases, plumes reach the scale of peripheral arctic seas, and amplification is expected during upcoming decades. Conclusions are mapped from the Lena to other boreal discharges, and future research questions are outlined regarding the bonding type versus mass release as permafrost degrades. Dynamic aqueous organic coupling is recommended for polar system models, from headwaters to coastal diluent.

54 ENVIRONMENTAL SCIENCES↗

Dual-frequency (Ka-band and G-band) radar estimates of liquid water content profiles in shallow clouds

The profile of the liquid water content (LWC) in clouds provides fundamental information for understanding the internal structure of clouds, their radiative effects, propensity to precipitate, and degree of entrainment and mixing with the surrounding environment. In principle, differential absorption techniques based on coincident dual-frequency radar reflectivity observations have the potential to provide the LWC profile. Previous differential frequency radar reflectivity (DFR) efforts were challenged by the fact that the measurable differential attenuation for small quantities of LWC is usually comparable to the system measurement error. This typically renders the retrieval impractical, as the uncertainty can become many times greater than the retrieved value itself. Theoretically, this drawback can be mitigated following two interconnected approaches: (1) increasing the frequency separation between the dual-frequency radar system to measure greater differential attenuation and (2) increasing the radar operating frequency to reduce the instrument measurement random error. Our recently developed 239 GHz radar was deployed during the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE) along with a variety of collocated remote sensing and in situ instruments. We have combined Ka-band (35 GHz) and G-band (239 GHz) observations to retrieve the LWC from more than 100 vertical profiles of shallow clouds with typical amounts of LWC smaller than 1 g m -3 . We theoretically and experimentally demonstrate that the Ka-band and G-band pair of frequencies offers at least a 65 % relative improvement in the LWC retrieval sensitivity compared to previous works reported in the literature using lower-frequency radars. This new technique provides a missing capability to determine the LWC in the challenging low liquid water path (LWP) range (< 200 g m -2 ) and suggests a way forward to characterize microphysical and dynamical processes more precisely in shallow clouds.

54 ENVIRONMENTAL SCIENCES↗