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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

COMBLE Radar b1 Processing: Corrections, Calibrations, and Processing Report

The U.S. Department of Energy’s (DOE) Atmospheric Radiation Measurement (ARM) user facility recently concluded its Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE), with its campaign emphasis on marine boundary-layer clouds and mixed-phase clouds during cold-air outbreaks. The COMBLE campaign featured the deployment of the first ARM Mobile Facility (AMF1) to northern Scandinavia (Andenes, Norway), including its standard complement of ARM cloud radars. In keeping with user demands stemming from the previous AMF Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign in Argentina, a post-campaign radar mentor effort was initiated for COMBLE. This activity was intended to improve the usability of the ARM cloud radar data sets in response to overall demands for calibrated, corrected data sets for downstream studies and retrieval applications. In addition to the terrain complexities previously important to CACTI data sets (e.g., clutter designation and/or removal), COMBLE presented new challenges to existing ARM radar mentor capabilities. These included the extension of existing methodologies (e.g., relative calibration adjustment [RCA] target techniques) to frozen environments and the potential issues with their applicability when considering mixed-phase precipitation conditions. As in the previous CACTI documentation (Hardin et al. 2020), the overall calibration and conditioning process in ARM nomenclature is referred to as generating a “b1” datastream. For the radars, these “b1” standards refer to a datastream that has been calibrated (and cross-calibrated), with effort to deliver the highest-quality (well-characterized) data possible. The “b1” radar mentor reporting (this current document) is intended to detail (i) the status/quality of the original “a1” (raw) data sets during the COMBLE AMF campaign, (ii) the corrections and calibrations that are applied to generate the b1 datastreams available on ARM’s Data Discovery, and (iii) the details of the applied methods, e.g., how radar offset/calibration numbers were determined.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

A Comprehensive Northern Hemisphere Particle Microphysics Data Set From the Precipitation Imaging Package

Microphysical observations of precipitating particles are critical data sources for numerical weather prediction models and remote sensing retrieval algorithms. However, obtaining coherent data sets of particle microphysics is challenging as they are often unindexed, distributed across disparate institutions, and have not undergone a uniform quality control process. This work introduces a unified, comprehensive Northern Hemisphere particle microphysical data set from the National Aeronautics and Space Administration precipitation imaging package (PIP), accessible in a standardized data format and stored in a centralized, public repository. Data is collected from 10 measurement sites spanning 34° latitude (37°N–71°N) over 10 years (2014–2023), which comprise a set of 1,070,000 precipitating minutes. The provided data set includes measurements of a suite of microphysical attributes for both rain and snow, including distributions of particle size, vertical velocity, and effective density, along with higher-order products including an approximation of volume-weighted equivalent particle densities, liquid equivalent snowfall, and rainfall rate estimates. The data underwent a rigorous standardization and quality assurance process to filter out erroneous observations to produce a self-describing, scalable, and achievable data set. Case study analyses demonstrate the capabilities of the data set in identifying physical processes like precipitation phase-changes at high temporal resolution. Bulk precipitation characteristics from a multi-site intercomparison also highlight distinct microphysical properties unique to each location. This curated PIP data set is a robust database of high-quality particle microphysical observations for constraining future precipitation retrieval algorithms, and offers new insights toward better understanding regional and seasonal differences in bulk precipitation characteristics.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1981

Summary of the status of the Nimbus-7 SMMR

The present state of calibration of the Nimbus-7 SMMR is described, and its relevance to retrievals of sea surface temperatures is discussed. The asymmetry in the polarization rotation was studied by calibrating the SMMR signals without the polarization rotation correction within a data set consisting of about 300 orbits, and the phase shift was determined by regression analysis. The largest phase shift was observed in the 1.4 cm vertical polarization channel - almost 11 degrees. The in-orbit calibration adjustment scheme is described, and the result of applying it to the 4.6 cm vertical polarization channel is shown.

Gloersen, P.↗
NASA NTRSDate not supplied

The View From Out Here: The Solar System Planets as Exoplanet Analogs

As we begin to characterize planets orbiting other stars, one of the most important tools available to us is the collection of disk-integrated solar system observations. To date, these have been limited in how they match up with expected exoplanet observations in terms of wavelength, time, viewing geometry, and separations. The Interstellar Probe mission could push the boundaries of planetary science by providing a much-needed and unique dataset for the solar system viewed as an extrasolar system in advance of the next generation of ground and space-based telescopes. Viewing the solar system at large separations over a long period serves several purposes. It acts as a practical test directly analogous to exoplanet observations under realistic conditions, including such effects as zodiacal dust (e.g., Roberge et al., 2012). Secondly, it allows for both the validation of forward models (that is, simulating a planet and generating spectra) and retrievals (where some of the planetary properties are not known) (e.g., Robinson et al., 2011; Agarwal and Wettlaufer, 2017). Third, the mission pro le would be able to collect data at both high- and low-phase angles, which are lacking for most of the solar system planets (e.g., Mallama and Hilton, 2018). Lastly, the long duration of the proposed mission would allow not only snapshots, but time resolved observations using the same instrument, highlighting the dynamic nature of the planets (e.g., seasonality, storms). The planets need not be resolved to make these observations, which eases instrumentation requirements. Here, we show simulations of what an Interstellar Probe imager would see, improving on work that was part of a white paper submitted to the Planetary Science and Astrobiology Decadal Survey. The opportunity for multiple full orbits for most of the solar system planets, including a full phase curve of Saturn, is unique and worth pursuing during the development of the Interstellar Probe mission.

Chester Harman↗
DOE OSTI2020

Impact of Cloud Longwave Scattering on Radiative Fluxes Associated With the Madden-Julian Oscillation in the Indian Ocean and Maritime Continent

Previous studies suggested that cloud longwave radiation contributes to the development and maintenance of the Madden-Julian Oscillation (MJO) and model-based convection is highly sensitive to the radiation scheme. However, currently used radiation schemes do not take cloud longwave scattering into account, resulting in an overestimation of the outgoing longwave radiation (OLR) and an underestimation of the downward longwave flux at the surface. We use combined active and passive satellite cloud property retrievals to quantify the one-layer cloud OLR and heating rate (HR) biases introduced by neglecting cloud longwave scattering in the Indian Ocean and Maritime Continent in the context of MJO, with a focus on its phases 3, 5, and 6. Here, the results show that the satellite-detected one-layer cloud area consists primarily of ice clouds, particularly during the boreal winter in the 4-year study period. An increased ice cloud area fraction of one-layer cloud groups is present up to 5 days before the onset of MJO events. If longwave scattering is neglected, the composite mean OLR overestimation over the one-layer ice cloud area from 5 days before to 4 days after the MJO passage is approximately 3.5 to 5.0 W m –2 . Neglecting longwave scattering also leads to a HR underestimation at cloud base and an overestimation at cloud top, making the base-to-top heating gradient less sharp at the cloud-resolving scale.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2019

Robotic Mars Sample Return and Earth entry vehicle concept development

NASA has studied potential Mars Sample Return over many decades, and the most recent Planetary Science Decadal Survey recommended making significant progress on this topic one of its highest priority goals. Recent inter-agency discussions and scientific support are lending credence to current Mars Sample Return planning activities, which notionally target launch of Sample Retrieval Lander and Earth Return Orbiter flight elements in 2026, and return of Martian samples to Earth in 2031. As part of the Mars Sample Return architecture under consideration, an Earth Entry Vehicle would perform the final phase by protecting the samples through severe entry environments using a 60-deg. sphere-cone flying on a passive/ballistic trajectory. The Earth Entry Vehicle design activities in particular are considering a variety of potential challenges, including: minimizing vehicle mass due to the need to travel to Mars and back to Earth, vehicle robustness to Micrometeroid and Orbital Debris impacts, capability to withstand severe entry environments while minimizing landing ellipse size, and providing impact load attenuation during a high-speed landing to meet Martian sample tube load limits and ensure sample containment in off-nominal scenarios. The present work provides a snapshot of current study work in progress, and highlights paths being taken to address these various design challenges for the conceptual Earth Entry Vehicle.

Corliss, James↗
NASA NTRSDate not supplied

PlanetarY Telemetric Helicopter for Investigation and Analysis (PYTHIA): A Rotorcraft for Martian Lava Tube Exploration

The PlanetarY Telemetric Helicopter for Investigation and Analysis (PYTHIA) project presents an early feasibility study into future Mars rotorcraft. With the success of Ingenuity and the current development of the Mars Sample Retrieval Helicopters, there is motivation to explore additional vehicle concepts for Mars exploration. This work presents an early conceptual design of a lava tube exploring quadrotor. The nominal mission for the PYTHIA quadrotor includes a two-phase in-depth exploration of one or mutliple lava tubes in the area of interest, Arsia Mons. A sizing analysis was completed using the NASA Design and Analysis of Rotorcraft (NDARC) tool. An eight-bladed quadrotor was selected based on the NDARC sizing sweeps. With preliminary vehicle and blade sizing completed, a flow visualization study was conducted. Two simulations were completed in Rotorcraft Computational Fluid Dynamics (RotCFD): one of the quadrotor alone and another in a lava tube. This paper introduces a baseline reference mission, preliminary vehicle design, and initial sizing analysis of a rotorcraft to explore Martian lava tubes.

PlanetarY↗
DOE OSTI2021

p +p - electroproduction off protons in deuterium: measurements of quasi-free cross sections and kinematic probing of final state interactions

In this study, the process of pi+pi- electroproduction off protons bound in deuterium nuclei is explored. The exploration is performed through the analysis of experimental data on electron scattering off the deuteron target, collected in Hall B at Jefferson Lab with the CLAS detector. As a main result, the set of integrated and single-differential cross sections of the reaction yvp(n) -> p'(n')pi+pi- is obtained. The cross sections are extracted in the quasi-free regime, which implies that only events not affected by final state interactions are subject to selection. The measurements are performed in the kinematic region of the invariant mass W from 1.3 GeV to 1.825 GeV and photon virtuality Q2 from 0.4 GeV2 to 1 GeV2. Sufficient experimental statistics allows narrow binning, i.e. 25 MeV in W and 0.05 GeV2 in Q2, while maintaining an adequate statistical uncertainty. The extraction of quasi-free cross sections is accompanied by the kinematic probing of FSI between the reaction final hadrons and the spectator neutron in the aforementioned exclusive channel. In this probing the distributions of missing quantities are used in order to investigate the relative spread of events with FSI along the reaction phase space, trace the difference of FSI manifestations in different reaction topologies, reveal details on alterations of the hadron momentum in FSI, and isolate FSI contributions of various final hadrons. The performed examination is also capable of retrieving information on some underlying FSI mechanisms, among which the process of resonance formation in the intermediate state of pion-neutron interactions is particularly remarkable.

Skorodumina, Iuliia↗
NASA NTRS1991

Measured space environmental effects to LDEF during retrieval

The Interim Operational Contamination Monitor (IOCM) is an attached shuttle payload to the Long Duration Exposure Facility (LDEF) that was used on 2 earlier flights to quantify the contamination deposited during the course of the missions. The IOCM can characterize by direct measurement the deposition of molecular and particulate contamination during any phase of flight. Also, the IOCM actively measures the optical property changes of thermal control surfaces by calorimetry, the flux of the ambient atomic oxygen environment, the incident solar flux, and the absolute ambient pressure in the payload bay. The IOCM also provides a structure and sample holders for the exposure of passive material samples to the space environment, e.g., thermal cycling, atomic oxygen, and micrometeoroids and/or debris. Some of the more salient results from the flight suggests that the payload bay was slightly contaminated during both the prelaunch phase of the mission and after the deployment of the SYNCOM IV payload. Measurements during the postflight phases, i.e., ferry flight and deintegration processing, show negligible to very low mass deposition. The results of the data are discussed in depth.

Maag, Carl R.↗
NASA NTRS2001

Latent Heating Retrievals Using the TRMM Precipitation Radar: A Multi-Seasonal Study

Rainfall is a key link in the hydrologic cycle and is a primary heat source for the atmosphere. The vertical distribution of latent heat release, which is accompanied by rainfall, modulates the large-scale circulations of the tropics and in turn can impact midlatitude weather. This latent heat release is a consequence of phase changes between vapor, liquid, and solid water. Present largescale weather and climate models can simulate latent heat release only crudely, thus reducing their confidence in predictions on both global and regional scales. This paper represents the first attempt to use NASA Tropical Rainfall Measuring Mission (TRMM) rainfall information to estimate the four-dimensional structure of global monthly latent heating profiles over the global tropics from December 1997 to October 2000. The Goddard Convective-Stratiform. Heating (CSH) algorithm and TRMM precipitation radar data are used for this study. We will examine and compare the latent heating structures between 1997-1998 (winter) ENSO and 1998-2000 (non-ENSO). We will also examine over the tropics. The seasonal variation of heating over various geographic locations (i.e., oceanic vs continental; Indian oceans vs west Pacific; Africa vs S. America) will be also examined and compared. In addition, we will examine the relationship between latent heating (max heating level) and SST. The period of interest also coincides with several TRMM field campaigns that recently occurred over the South China Sea in 1998 (SCSMEX), Brazil in 1999 (TRMM-LBA), and in the central Pacific in 1999 (KWAJEX). Sounding diagnosed Q1 budgets from these experiments could provide a means of validating the retrieved profiles of latent heating from the CSH algorithm.

Tao, Wei-Kuo↗
NASA NTRS2011

Multiangle Implementation of Atmospheric Correction (MAIAC):: Radiative Transfer Basis and Look-up Tables - 1

This paper describes a radiative transfer basis of the algorithm MAIAC which performs simultaneous retrievals of atmospheric aerosol and bidirectional surface reflectance from the Moderate Resolution Imaging Spectroradiometer (MODIS). The retrievals are based on an accurate semianalytical solution for the top-of-atmosphere reflectance expressed as an explicit function of three parameters of the Ross-Thick Li-Sparse model of surface bidirectional reflectance. This solution depends on certain functions of atmospheric properties and geometry which are precomputed in the look-up table (LUT). This paper further considers correction of the LUT functions for variations of surface pressure/height and of atmospheric water vapor, which is a common task in the operational remote sensing. It introduces a new analytical method for the water vapor correction of the multiple ]scattering path radiance. It also summarizes the few basic principles that provide a high efficiency and accuracy of the LUT ]based radiative transfer for the aerosol/surface retrievals and optimize the size of LUT. For example, the single-scattering path radiance is calculated analytically for a given surface pressure and atmospheric water vapor. The same is true for the direct surface-reflected radiance, which along with the single-scattering path radiance largely defines the angular dependence of measurements. For these calculations, the aerosol phase functions and kernels of the surface bidirectional reflectance model are precalculated at a high angular resolution. The other radiative transfer functions depend rather smoothly on angles because of multiple scattering and can be calculated at coarser angular resolution to reduce the LUT size. At the same time, this resolution should be high enough to use the nearest neighbor geometry angles to avoid costly three ]dimensional interpolation. The pressure correction is implemented via linear interpolation between two LUTs computed for the standard and reduced pressure levels. A linear mixture and a modified linear mixture methods are used to represent different aerosol types in the aerosol/surface retrievals from several base models of the fine and coarse aerosol fractions. In summary, the developed LUT algorithm allows fast high-accuracy simulations of the outgoing radiance with full variability of the atmospheric and surface bidirectional reflectance properties for the aerosol/surface remote sensing.

Lyapustin, Alexei↗
DOE OSTI2023

Deep Learning Parameterization of Vertical Wind Velocity Variability via Constrained Adversarial Training

Atmospheric models with typical resolution in the tenths of kilometers cannot resolve the dynamics of air parcel ascent, which varies on scales ranging from tens to hundreds of meters. Small-scale wind fluctuations are thus characterized by a subgrid distribution of vertical wind velocity W with standard deviation σ W . The parameterization of σ W is fundamental to the representation of aerosol–cloud interactions, yet it is poorly constrained. Using a novel deep learning technique, this work develops a new parameterization for σ W merging data from global storm-resolving model simulations, high-frequency retrievals of W , and climate reanalysis products. The parameterization reproduces the observed statistics of σ W and leverages learned physical relations from the model simulations to guide extrapolation beyond the observed domain. Incorporating observational data during the training phase was found to be critical for its performance. The parameterization can be applied online within large-scale atmospheric models, or offline using output from weather forecasting and reanalysis products.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

X-Band Scanning ARM Precipitation Radar, CF/Radial Formatted, Quality Controlled

The X-band Scanning ARM Precipitation Radar (X-SAPR) is an X-band dual-polarization Doppler weather radar. The X-SAPR operates in a simultaneous transmit and receive (STAR) mode, meaning that the transmit signal is split so that power is transmitted on both horizontal and vertical polarizations at the same time. The X-SAPR transmitter is a 200 kW (peak power) magnetron. The receiver is based upon the Vaisala RVP-900 and runs Vaisala’s IRIS software. In addition to the first three Doppler moments (reflectivity, radial velocity, and spectra width), the X-SAPR also provides differential reflectivity, correlation coefficient, and specific differential phases. The dual-polarization variables enable estimates of rainfall rates and identification of precipitation types. At the Southern Great Plains site, three X-SAPRs surround the Central Facility, allowing the use of multi-Doppler velocity retrievals to estimate wind fields.

xsaprcfrqc↗
NASA NTRS1989

The astronaut and the banana peel: An EVA retriever scenario

To prepare for the problem of accidents in Space Station activities, the Extravehicular Activity Retriever (EVAR) robot is being constructed, whose purpose is to retrieve astronauts and tools that float free of the Space Station. Advanced Decision Systems is at the beginning of a project to develop research software capable of guiding EVAR through the retrieval process. This involves addressing problems in machine vision, dexterous manipulation, real time construction of programs via speech input, and reactive execution of plans despite the mishaps and unexpected conditions that arise in uncontrolled domains. The problem analysis phase of this work is presented. An EVAR scenario is used to elucidate major domain and technical problems. An overview of the technical approach to prototyping an EVAR system is also presented.

Shapiro, Daniel G.↗
NASA NTRS1992

Lidar Studies of Extinction in Clouds in the ECLIPS Project

The Experimental Cloud Lidar Pilot Study (ECLIPS) project has now had two active phases in 1989 and 1991. A number of laboratories around the world have taken part in the study. The observations have yielded new data on cloud height and structure, and have yielded some useful new information on the retrieval of cloud optical properties, together with the uncertainties involved. Clouds have a major impact on the climate of the earth. They have the effect of reducing the mean surface temperature from 30 C for a cloudless planet to a value of about 15 C for present cloud conditions. However, it is not at all certain how clouds would react to a change in the planetary temperature in the event of climate change due to a radiative forcing from greenhouse gases. Clouds both reflect out sunlight (negative feedback) and enhance the greenhouse effect (positive feedback), but the ultimate sign of cloud feedback is unknown. Because of these uncertainties, campaigns to study clouds intensely were initiated. The International Satellite Cloud Climatology (ISCPP) and the FIRE Campaigns (cirrus and stratocumulus) are examples. The ECLIPS was set up similarly to the above experiments to obtain information specifically on cloud base, but also cloud top (where possible), optical properties, and cloud structure. ECLIPS was designed to allow as many laboratories as possible globally to take part to get the largest range of clouds. It involves observations with elastic backscatter lidar, supported by infrared fluxes at the ground and radiosonde data, as basic instrumentation. More complex experiments using beam filter radiometers, solar pyranometers, and satellite data and often associated with other campaigns were also encouraged to join ECLIPS. Two periods for observation were chosen, Sep. - Dec. 1989 and Apr. - Jul. 1992 into which investigators were requested to fit 30 days of observations. These would be either continuous, or arranged to coincide with NOAA satellite overpasses to obtain AVHRR data. The distribution of the ECLIPS international effort as in 1991 is shown. The main gaps in the global distribution are in the tropics and the Southern Hemisphere.

Martin, C.↗
NASA NTRS2008

Effect of the Inhomogeneity of Ice Crystals on Retrieving Ice Cloud Optical Thickness and Effective Particle Size

Spherical or spheroidal air bubbles are generally trapped in the formation of rapidly growing ice crystals. In this study the single-scattering properties of inhomogeneous ice crystals containing air bubbles are investigated. Specifically, a computational model based on an improved geometric-optics method (IGOM) has been developed to simulate the scattering of light by randomly oriented hexagonal ice crystals containing spherical or spheroidal air bubbles. A combination of the ray-tracing technique and the Monte Carlo method is used. The effect of the air bubbles within ice crystals is to smooth the phase functions, diminish the 22deg and 46deg halo peaks, and substantially reduce the backscatter relative to bubble-free particles. These features vary with the number, sizes, locations and shapes of the air bubbles within ice crystals. Moreover, the asymmetry factors of inhomogeneous ice crystals decrease as the volume of air bubbles increases. Cloud reflectance lookup tables were generated at wavelengths 0.65 m and 2.13 m with different air-bubble conditions to examine the impact of the bubbles on retrieving ice cloud optical thickness and effective particle size. The reflectances simulated for inhomogeneous ice crystals are slightly larger than those computed for homogenous ice crystals at a wavelength of 0.65 microns. Thus, the retrieved cloud optical thicknesses are reduced by employing inhomogeneous ice cloud models. At a wavelength of 2.13 microns, including air bubbles in ice cloud models may also increase the reflectance. This effect implies that the retrieved effective particle sizes for inhomogeneous ice crystals are larger than those retrieved for homogeneous ice crystals, particularly, in the case of large air bubbles.

Xie, Yu↗
NASA NTRS2013

Estimating the Concentration of Large Raindrops from Polarimetric Radar and Disdrometer Observations

Estimation of rainfall integral parameters, including radar observables, and empirical relations between them are sensitive to the truncation of the drop size distribution (DSD), particularly at the large drop end. The sensitivity of rainfall integral parameters to the maximum drop diameter (D(sub max)) is exacerbated at C‐band since resonance effects are pronounced for large drops in excess of 5 mm diameter (D). Due to sampling limitations, it is often difficult to reliably estimate D(sub max) with disdrometers. The resulting uncertainties in D(sub max0 potentially increase errors in radar retrieval methods, particularly at C‐band, that rely on disdrometer observations for DSD input to radar models. In fact, D(sub max) is typically an assumed DSD parameter in the development of radar retrieval methods. Because of these very uncertainties, it is difficult to independently confirm disdrometer estimates of D(sub max) with polarimetric radar observations. A couple of approaches can be taken to reduce uncertainty in large drop measurement. Longer integration times can be used for the collection of larger disdrometer samples. However, integration periods must be consistent with a radar resolution volume (RRV) and the temporal and spatial scales of the physical processes affecting the DSD therein. Multiple co‐located disdrometers can be combined into a network to increase the sample size within a RRV. However, over a reasonable integration period, a single disdrometer sample volume is many orders of magnitudes less than a RRV so it is not practical to devise a network of disdrometers that has an equivalent volume to a typical RRV. Since knowledge of DSD heterogeneity and large drop occurrence in time and space is lacking, the specific accuracy or even general representativeness of disdrometer based D(sub max) and large drop concentration estimates within a RRV are currently unknown. To address this complex issue, we begin with a simpler question. Is the frequency of occurrence of large rain drops (D > 5 mm) in disdrometer observations, either stand alone or networked, generally representative and consistent with polarimetric radar observations? We first show from simulations that the concentration of large (D > 5 mm) rain drops (N(sub T5)) can be estimated from polarimetric observations of specific differential phase (K(sub dp)) and differential reflectivity (Z(sub dr)), N(sub T5)=F(K(sub dp),Z(sub dr)), or horizontal reflectivity (Z(sub h)) and Z(sub dr), N(sub T5)=(Z(sub h),Z(sub dr)). We assess the error associated with polarimetric retrieval of N(sub T5), including sensitivity to D(sub max) parameterization assumptions and measurement error in the radar simulations. Polarimetric measurements at S‐band and C‐band will then be used to retrieve estimates of N(sub T5) and compared to disdrometer estimates of N(sub T5). After careful consideration of retrieval error, we will check consistency between disdrometer and polarimetric radar estimates of N(sub T5) and the frequency of occurrence of large rain drops in a variety of precipitating regimes using data from NASA's Global Precipitation Measurement (GPM) Ground Validation (GV) program, including field campaigns such as MC3E (Oklahoma) and IFloodS (Iowa) and extended measurements over Huntsville, Alabama and NASA Wallops Flight Facility in coastal Virginia.

Carey, Lawrence D.↗
DOE OSTI2020

Aerosol Optical Tweezers Elucidate the Chemistry, Acidity, Phase Separations, and Morphology of Atmospheric Microdroplets

Aerosol particles represent unique chemical environments because of their high surface area-to-volume ratio that promotes the effects of interfacial chemistry in confined environments. Properties such as viscosity, diffusivity, water content, pH, and morphology—following liquid–liquid phase separation—can strongly alter how a particle interacts with condensable vapors and reactive trace gases, thus modifying its continual evolution and environmental effects. Our understanding of this chemical evolution of atmospheric particulate matter and its environmental impacts is largely limited by our ability to directly observe how these critical particle properties respond to the addition or reactive uptake of new chemical components. Aerosol optical tweezers (AOT) stably trap particles in focused laser beams, providing positional control and the retrieval of many of these critical properties required to understand and predict the chemistry of aerosolized microdroplets. The analytical power of the AOT stems from the retrieval of the cavity-enhanced Raman spectrum induced by the trapping laser. Analysis of the whispering gallery modes (WGMs) that resonate as a standing wave around the droplet’s interface, provide high accuracy measurements of the droplet’s size, refractive index (and thus a measurement of composition), and can distinguish between core–shell, partially engulfed, and homogeneous morphologies. In this study, we have advanced the ability to determine the properties of the core and shell phases in biphasic droplets, including obtaining high-accuracy pH measurements. These capabilities were applied to perform AOT physical chemistry experiments on authentic secondary organic aerosol (SOA) produced directly in the AOT chamber by ozonolysis of terpene vapors. The propensity of the SOA to phase separate as a shell from a wide range of nonpolar to polar core phases was observed, along with the discovery of a stable emulsified state of SOA particles in an aqueous salt droplet. Micron-thick SOA shells did not impede the gain or loss of water or squalane from the core to the surrounding air, indicating no significant diffusional limitations to condensational growth or partitioning even under dry conditions. These experiments formed the foundation of a new framework that predicts how the phase-separated morphology of complex aerosols containing organic carbon evolves during continual atmospheric oxidation processes. Increases in oxidation state will quickly drive conversion from a partially engulfed to core–shell morphology that has dramatically different chemical reactivity since the core phase is completely concealed by the shell. The recent advances in the experimental capabilities of the AOT technique such as presented here enable novel experimental methodologies that provide insights into the chemistry and multidimensional properties of aerosol microdroplets, and how these coevolve and respond to continual chemical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗