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DOE OSTI2023

Hyperfine structure and isotope shifts of xenon measured for near-infrared transitions with Doppler-free saturated absorption spectroscopy

Hyperfine structure and isotope shifts of Xe were investigated with Doppler-free saturated absorption spectroscopy for all transitions in the 820-841 nm spectral interval. The Xe samples were commercial gases of natural isotopic abundances. The measurements were performed by employing a widely tunable narrow line Ti:sapphire laser. The hyperfine structures for 129 Xe and 131 Xe were well resolved. For the transitions with the wavelengths in vacuum near 820.860 nm and 841.150 nm also isotope shifts of the even isotopes were clearly observed. The modeling of the shapes of the observed absorption lines qualitatively reproduces experimental spectral profiles. The measured absorption peaks of the hyperfine structure and isotope shifts of Xe isotopes present characteristic spectral fingerprints for their identification. Eventually, quantitative spectral analysis will provide isotopic abundances of natural, as well as radioactive Xe gas samples.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Utilizing metal cation reactions with carbonyl sulfide to remove isobaric interferences in tandem inductively coupled plasma mass spectrometry analyses

Carbonyl sulfide (OCS) was used as a reaction gas to investigate gas phase metal (M + ) ion-molecule reactions using the Agilent 8900 inductively coupled plasma tandem mass spectrometer (ICP-MS/MS) to yield insight on how this gas may be used to remove isobaric interferences in analytical measurements. The experimental work was paired with density functional theory (DFT) calculations of the reaction enthalpy to predict whether M + will react with OCS. A multi-element standard containing 46 elements ranging from 9 to 208 u was analyzed in the presence and absence of OCS. When a reaction was observed, the dominant product was the sulfide (MS + ). Oxide products were also observed for many M + but formation was less efficient with OCS than previously observed with other reaction gases. This is likely due to the weaker OC-S bond that makes MS + formation more favorable. Increasing the flow rate from 0.1 to 0.2 mL/min (corresponding to a change in reaction gas pressure from 0.35 to 0.53 Pa (2.6 to 4.0 mTorr)) generally resulted in greater MS + production, including the secondary product MS 2 + for a few cations. The early lanthanide series ions (La + , Ce + , Pr + and Nd + ) produced greater quantities of MO + at the higher pressure, although MS + products were still the dominant product. The DFT-predicted reaction enthalpies were consistent with the observed sulfide formation, with an accuracy >90%; however, model predictions were less accurate for the minor and higher order products (< 77% for MO + ). Finally, the work presented here continues a systematic study of ion-molecule reactions in ICP-MS/MS to understand and develop new and novel ways to analyze complex mixtures with minimal pre-analysis treatment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Optimizing aluminum oxide passivation layers—Laser-induced plasmas for layer formation, real-time diagnostics, and layer evaluation

Molten salts have beneficial thermophysical and electrolytic properties, but the aggressive nature of molten salts requires corrosion mitigation strategies, such as structural material surface treatment. In this study, a laser-induced breakdown spectroscopy (LIBS) system was used to simultaneously ablate and monitor de-excitation spectra to form and identify dense alumina passivation layers. Additionally, high-frequency (kHz) LIBS imaging allowed rapid elemental mapping and depth profiling for surface O/Al ratios via minimally destructive analysis. The paired t-test rejected the null hypothesis that air and Ar cover gases were equivalent (p = 0.00012), and the analysis of variance (ANOVA) showed that overlap between shots (p = 0.03112) and cover gas flow rate (p = 0.02729) were statistically significant. At 75% overlap, the O/Al ratio increased to 10% ± 2%, and 90% overlap rose further to 31% ± 2%. Regardless of overlap, tuning the gas flow from 0.5 to 2.5 L min −1 enhanced the O/Al ratio by 24% ± 4%. LIBS depth profiling showed a 3× increase in layer thickness from 75% to 90% overlap. Molecular band peaks of AlO, a precursor to Al 2 O 3 found during treatment, suggest that band intensity could be used for real-time Al 2 O 3 optimization. Ultimately, by adjusting laser spot overlap and cover gas flow rate, a 266 nm laser was shown to form Al 2 O 3 layers on an Al6061 sample, with cover gas flow rate primarily affecting the O/Al ratio and layer thickness correlating with laser spot overlap. This combination of molecular spectra collection, imaging, and depth profiling demonstrated the robust layer analysis capabilities of LIBS.

Corrosion↗

DOE OSTI2023

Climate effects of future aerosol reductions for achieving carbon neutrality in China

To limit the global warming to 1.5 °C above pre-industrial levels, beyond which the most dangerous impacts of climate change will occur, achieving carbon neutrality by the mid-21st century is essential. As the largest developing country and a significant contributor to carbon dioxide (CO 2 ) emissions, China has announced its ambitious climate commitment to pass carbon peak before 2030 and to achieve carbon neutrality by 2060. Both climate policies and regional clean air actions have been implemented for reductions in fossil fuel emissions, including the emissions of short-lived aerosols and precursors. Furthermore, in the context of pursuing carbon neutrality in China, aerosol reductions due to clean air actions and pollution control policies are very likely to have a great impact on climate. In this study, climate effects of aerosol reductions due to China's clean air actions under localized future emission scenarios are investigated using the Community Earth System Model version 1 (CESM1). Fully coupled and atmosphere-only experiments in years of carbon peak (2030) and carbon neutrality (2060) are performed with anthropogenic emissions of aerosols and precursors under “Current-goals” (Current) and “Carbon-Neutral” (Neutral) scenarios from the Dynamic Projection for Emissions in China (DPEC) model that consider socioeconomic development, climate policy, and pollution control actions (Figs. S1–S4 online). In addition, a present-day emissions simulation (PD) is conducted as the reference case (Supplementary materials online). Another sensitivity simulation is also conducted, with black carbon (BC) emissions set to follow the Neutral experiment but other emissions kept at the present-day levels (Neutral_BC), to quantify the relative roles of reducing strongly absorbing BC and other aerosols on future climate towards carbon neutrality. Greenhouse gases concentrations are kept at the 2015 levels in all simulations (Text S1 online).

Yang, Yang↗

DOE OSTI2023

Observed impacts of large wind farms on grassland carbon cycling

Deployment of wind energy is an essential renewable energy source that mitigates climate change and reduces air pollution. Over the last several decades, wind energy development has increased worldwide, expanding from ~20 to ~900 GW (gigawatt) during 2001-2022. Nonetheless, researchers have identified unintended consequences of wind energy on microclimate via turbine-altered surface-atmosphere exchanges of energy, momentum, mass, and trace gases. Based on multi-source observations and models, researchers also have drawn some conclusions that wind farms could warm the land surface, especially at night, at regional and continental scales. Consequently, altered microclimates at wind farms may affect vegetation productivity and carbon sequestration, two critically important ecosystem services related to carbon dynamics; however, such potential impacts and driving mechanisms remain poorly understood. Wind energy deployment is increasing globally to meet carbon neutrality goals, with upscaling of onshore wind power capacity projected to grow from 542 GW in 2018 to 1787 and 5044 GW by 2030 and 2050, respectively. Furthermore, increased demand for wind energy deployment may lead to much larger wind farms in open, expansive landscapes. In turn, a large array of geographically clustered wind turbines could collectively modify local microclimate and amplify turbine-atmosphere interactions, which, if large enough, may produce detectable impacts on ecosystem dynamics. Thus, identifying and quantifying the potential impacts of wind farms on carbon-related ecosystem services may facilitate sustainable wind energy development globally.

17 WIND ENERGY↗

DOE OSTI2020

Photochemical reactions on aerosols at West Antarctica: A molecular case-study of nitrate formation among sea salt aerosols

Environmental implications of climate change are complex and exhibit regional variations both within and between the polar regions. The increase of solar UV radiation flux over Antarctica due to stratospheric ozone depletion creates the optimal conditions for photochemical reactions on the snow. Modeling, laboratory, and indirect field studies suggest that snowpack process release gases to the atmosphere that can react on sea salt particles in remote regions such as Antarctica, modifying aerosol composition and physical properties of aerosols. Here, we present evidence of photochemical processing in West Antarctica aerosols using microscopic and chemical speciation of individual atmospheric particles. Individual aerosol particles collected at the Brazilian module Criosfera 1 were analyzed by scanning transmission X-ray microscopy with near edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS) combined with computer controlled scanning electron microscopy (CCSEM) with energy-dispersive X-ray (EDX) microanalysis. The displacement of chlorine relative to sodium was observed over most of the sea salt particles. Particles with a chemical composition consistent with NaCl-NO3 contributed up to 30% of atmospheric particles investigated. Overall, this study provides evidence that the snowpack and particulate nitrate photolysis should be considered in dynamic partition equilibrium in the troposphere. Finally, these findings may assist in reducing modeling uncertainties and present new insights into the aerosol chemical composition in the polar environment.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Influence of restored mussel reefs on denitrification in marine sediments

Globally we have lost the majority of shellfish reefs, with the concomitant loss of ecosystem services. Restoration provides opportunities to regain lost services and engage society in the wider ecosystem benefits of restoration. Previous research has demonstrated that the functional role of shellfish can be context dependent, and we therefore measured fluxes of nutrients and dissolved gases from four restored mussel reefs along a grain size gradient in New Zealand as a metric of success in ecosystem function. This globally novel research found that restored mussel reefs were successful in enhancing denitrification. Mussel reefs can therefore be important in reducing the risk of future eutrophication, but the importance of nutrient remineralisation varies in response to site conditions. These data show that mussel reef creation can quickly restore ecosystem function, but site selection to enhance specific services is important. Furthermore, this study provides evidence of a poorly realised ecosystem service provided by restored mussel beds that allows future restoration efforts to better target areas in order to have the largest impact on the removal of anthropogenic nitrogen.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Ultrafast and selective gas transport through highly ordered black phosphorene nanochannels

Two-dimensional (2D) materials bring a great opportunity to fabricate molecular sieving membranes that can potentially break the permeability-selectivity trade-off. Although 2D laminar membranes with interlayer nanochannels as molecular sieving channel were widely studied, for most of reported 2D laminar membranes, it is of a great challenge to fabricate highly ordered interlayer nanochannels for mass transport. Herein, we report a novel kind of black phosphorene membrane which is made from the stacking of highly ordered 2D black phosphorene nanoflakes. The as prepared black phosphorene membrane shows H 2 permeance > 1000 GPU and H 2 /CO 2 selectivity > 100 for H 2 /CO 2 mixed gas, demonstrating an extremely high gas separation performance. The DFT calculation results demonstrate that the interlayer galleries in the black phosphorene membrane allow the H 2 passing through easily while block the other gases with bigger kinetic diameters, matching well with the experimental findings. In conclusion, the present results indicate that the interlayer galleries in the black phosphorene membrane can be applied as molecular sieving channels for gas separation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Effect of post-deposition heat treatment on microstructure and mechanical properties of NASA HR-1 cold spray coatings

The primary goal of this work was to examine the impact of heat treatment on the evolution of microstructure and mechanical properties of NASA HR-1 cold spray coatings. Coatings were produced employing a high pressure cold spray system using N2 and He process gases and the effect of process gas and deposition temperature on the microstructure and mechanical properties of the coatings was examined. Microstructural characterization was performed using optical microscopy, scanning electron microscopy, micro X-ray computed tomography, and electron backscatter diffraction. NASA HR-1 coatings produced with He process gas exhibited improved plastic deformation and resulted in the lowest porosity compared to those deposited with N2 process gas. All coatings showed brittle failure with limited ductility in the as-deposited condition. Heat treatment of the NASA HR-1 cold spray coatings was performed at 550°C and 950°C for 1 h to improve the mechanical strength of the coatings. Heat treatment improved the particle bonding and enhanced the mechanical properties of the cold spray coatings. Heat treatment performed at 550°C resulted in higher mechanical strength of coatings, whereas the heat treatment performed at 950°C resulted in recrystallized microstructure and improved ductility of the coatings. However, heat treatment at 950°C resulted in forming the Eta (η) phase and Ni-Ti intermetallics in all the NASA HR-1 cold spray coatings. Here, the overall results suggest that using He as process gas contributed to reduced porosity and enhanced mechanical properties of the cold spray coatings.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2020

Formation and energetics of amorphous rare earth (RE) carbonates in the RE 2 O 3 –CO 2 –H 2 O system

Amorphous materials are of interest in the genesis of crystalline solids. They are often the first to precipitate from supersaturated solutions and are in the nanometer size range, transforming into a nanocrystalline metastable phase, and then to thermodynamically stable phases. One must seek knowledge of the composition, structure, thermodynamics, kinetics, and reaction pathways that relate the amorphous and crystalline phases. The subject of this study is the amorphous phases in the system RE 2 O 3 -CO 2 –H 2 O (RE- La, Nd, Dy,Yb). They were synthesized via direct precipitation and urea hydrolysis, and characterized by powder XRD, DTA with mass spectrometric analysis of the evolved gases. Phases have the non-stoichiometric composition RE 2 O 3 ·xCO 2 ·yH 2 O (1 < x < 3, 3 < y <7), which is different from that of crystalline simple carbonates and hydroxycarbonates. Thus we consider them to be amorphous precursors, rather than amorphous carbonates. High temperature oxide melt solution calorimetry in molten sodium molybdate solvent was used to derive their enthalpies of formation from oxides and elements. Increase of energetic stability per mole of RE 2 O 3 compounds occurs in the order: RE 2 O 3 → 2RE(OH)3→ 2REO(OH) → RE 2 O 2 CO 3 → Amorphous precursor → 2(REOHCO 3 ) → RE 2 (CO 3 ) 3 ·yH 2 O. We calculated the enthalpies of possible transformations of amorphous precursors to crystalline phases and conclude that thermodynamics determines the dependence of the crystallizing products on the temperature and partial pressure of CO 2 and H 2 O. Amorphous precursors are clearly intermediate in the synthesis, and ternary phases containing both H 2 O and CO 2 compete with each other in terms of thermodynamic stability. The energy landscape obtained here will allow one to directly synthesize specific products and control their functionality.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

The role of infrastructure to enable and support electric drive vehicles: A Transportation Research Part D Special Issue

Widespread vehicle electrification appears to be necessary to achieve timely and deep reductions in greenhouse gases (GHG) and pollutant emissions as well as petroleum use in the transportation sector. The lack of a sufficient refuelling infrastructure has defeated many past efforts to promote alternatives to petroleum fuels. The papers in this special issue on the “Role of Infrastructure to Enable and Support Electric Drive Vehicles” address the diverse challenges posed by a transition from fossil-fuelled internal combustion engine vehicles to vehicles powered by electric motors and the special role of refuelling/recharging infrastructure in this transition. Electric drive vehicles are herein considered to be plug-in electric vehicles (PEVs), including plug-in hybrid electric vehicles (PHEVs), battery electric vehicles (BEVs), and hydrogen fuel cell electric vehicles (FCEVs). BEVs and FCEVs are also known as Zero Emission Vehicles (ZEVs) because their propulsion systems produce no tailpipe emissions.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2021

Molten-salt-mediated carbon dioxide capture and superequilibrium utilization with ethane oxidative dehydrogenation

Existing CO 2 -mediated oxidative dehydrogenation (CO 2 -ODH) of ethane has yet to demonstrate >60% single-pass CO yield due to the intrinsic equilibrium limitations. We report a unique approach with mixed molten carbonates as a reaction medium for CO 2 -ODH, which strategically partitions the CO 2 -ODH reactions into gas and molten-salt phases and facilitates integrated CO 2 capture from power plant flue gases. An 89% CO yield was achieved at 770°C, doubling the equilibrium limitation of conventional CO 2 -ODH. The high CO yield in turn enhances ethylene formation. Further characterizations confirmed that molten-salt mediated ODH (MM-ODH) proceeds through a gas-phase cracking and molten-salt mediated reverse water-gas-shift reaction pathway. Based on this understanding, thermodynamic analysis and ab initio molecular dynamics simulations were conducted to develop general principles to optimize the molten-salt reaction medium. Process analyses confirm that MM-ODH has the potential to be significantly more efficient for CO 2 capture and utilization than conventional CO 2 -ODH.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Production of β-ketoadipic acid from glucose in Pseudomonas putida KT2440 for use in performance-advantaged nylons

Biomass-derived chemicals can offer unique chemical functionality relative to petroleum-derived building blocks. To this end, here we report that β-ketoadipic acid (βKA), a C6 diacid with a β-ketone group, can be used as a performance-advantaged replacement for adipic acid in a nylon-6,6 analog. Building on our previous efforts to produce shikimate-derived products from carbohydrates, Pseudomonas putida KT2440 is engineered to produce βKA from glucose, achieving a 26 g/L titer. Following purification, βKA imparts an increase of 69 degrees C above the nylon-6,6 glass transition temperature and 20% reduced water permeability, equivalent to nylon-6,10. Molecular simulations predict that the enhanced thermal properties result from rigidity introduced by the β-ketone. Process analysis predicts that βKA can be produced for US$1.94/kg from sugars, requiring 63% less energy and emitting 43% less greenhouse gases than fossil-based adipic acid. Overall, this study illustrates the potential for βKA to serve as a useful building block for bio-based polymers.

09 BIOMASS FUELS↗

DOE OSTI2025

Harnessing nanoscale densification for controlling gas selectivity in flexible zeolitic imidazolate frameworks

Flexible metal-organic frameworks (MOFs) are promising for gas separation due to their molecular recognition capabilities. However, gate-opening behavior in certain flexible MOFs can reduce gas selectivity, enabling simultaneous adsorption of multiple gases. We introduce a binder-free, pressure-free densification process to enhance gas selectivity in flexible zeolitic imidazolate frameworks (ZIF-7 and ZIF-9) by optimizing nanoparticle packing. Unlike powders, the densified ZIF-7 and ZIF-9 retain rhombohedral crystal structures after solvent removal, confirmed via synchrotron powder X-ray diffraction. This process modifies adsorption behavior by introducing a diffusion barrier, enabling diffusivity-driven kinetic separation and enhanced CO2/hydrocarbon selectivity. At 0.5 bar, ZIF-7 mono shows 2×, 4×, and 9.5× higher CO 2 selectivity over C 2 H 2 , C 2 H 4 , and C 2 H 6 , respectively, versus ZIF-7 pwd . ZIF-9 mono similarly shows 6.5×, 3×, and 39× improvements over ZIF-9 pwd . Both monoliths outperform powders in ternary gas mixtures. This study provides a novel strategy to control gate opening and enhance gas selectivity in flexible MOFs for practical separation applications.

CO2/hydrocarbon separation↗

DOE OSTI2020

Development of a clostridia-based cell-free system for prototyping genetic parts and metabolic pathways

Gas fermentation by autotrophic bacteria, such as clostridia, offers a sustainable path to numerous bioproducts from a range of local, highly abundant, waste and low-cost feedstocks, such as industrial flue gases or syngas generated from biomass or municipal waste. Unfortunately, designing and engineering clostridia remains laborious and slow. The ability to prototype individual genetic part function, gene expression patterns, and biosynthetic pathway performance in vitro before implementing designs in cells could help address these bottlenecks by speeding up design. Unfortunately, a high-yielding cell-free gene expression (CFE) system from clostridia has yet to be developed. Here in this paper, we report the development and optimization of a high-yielding (236 ± 24 μg/mL) batch CFE platform from the industrially relevant anaerobe, Clostridium autoethanogenum. A key feature of the platform is that both circular and linear DNA templates can be applied directly to the CFE reaction to program protein synthesis. We demonstrate the ability to prototype gene expression, and quantitatively map aerobic cell-free metabolism in lysates from this system. We anticipate that the C. autoethanogenum CFE platform will not only expand the protein synthesis toolkit for synthetic biology, but also serve as a platform in expediting the screening and prototyping of gene regulatory elements in non-model, industrially relevant microbes.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Time-resolved particle image velocimetry measurements of the turbulent Richtmyer–Meshkov instability

Experiments are presented on the Richtmyer–Meshkov instability (RMI) with a three-dimensional, multi-mode initial perturbation. The experiments use a vertical shock tube, where a stably stratified interface is formed between air and sulphur hexafluoride (SF 6 ) via counterflow. A perturbation is imposed at the interface by vertical oscillation of the gas column, forming Faraday waves. The interface is accelerated by a Mach 1.17 (in air) shock wave, and the development of the mixing region between the gases is investigated using particle image velocimetry. Following shock acceleration, a reflected shock wave from the bottom of the shock tube interacts with the mixing layer a second time (reshock). The experiment is initialized with both high and low amplitude perturbations to examine the effect of the perturbation amplitude on measured quantities. The instability growth exponent (θ) is determined from the kinetic energy field using the width of the mixing layer and the decay of kinetic energy, which are found to be in agreement when the flow is most strongly excited. A growth exponent of θ ≈ 0.5 is found for all cases except the high-amplitude reshocked regime (where θ ≈ 0.33). High-amplitude experiments exhibit the transitional outer Reynolds number (Re ≡ hh˙/ν >10 4 ) required for mixing transition following the incident shock, and both experiments are elevated well above this threshold following reshock. However, neither set of experiments meet the more stringent requirements proposed by Zhou et al. (Phys. Rev.E, vol. 67, issue 5, 2003) which include the time dependent aspect of the RMI, an observation which is also made when examining the spectra.

42 ENGINEERING↗

DOE OSTI2025

A moment-conserving discontinuous Galerkin representation of the relativistic Maxwellian distribution

Kinetic simulations of relativistic gases and plasmas are critical for understanding diverse astrophysical and terrestrial systems, but the accurate construction of the relativistic Maxwellian, the Maxwell–Jüttner distribution, on a discrete simulation grid is challenging. Difficulties arise from the finite velocity bounds of the domain, which may not capture the entire distribution function, as well as errors introduced by projecting the function onto a discrete grid. Here, we present a novel scheme for iteratively correcting the moments of the projected distribution applicable to all grid-based discretizations of the relativistic kinetic equation. In addition, we describe how to compute the needed nonlinear quantities, such as Lorentz boost factors, in a discontinuous Galerkin scheme through a combination of numerical quadrature and weak operations. The resulting method accurately captures the distribution function and ensures that the moments match the desired values to machine precision.

astrophysical plasmas↗

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↗