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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

The Significant Role of New Particle Composition and Morphology on the HNO 3 -Driven Growth of Particles down to Sub-10 nm

New particle formation and growth greatly influence air quality and the global climate. Recent CERN Cosmics Leaving OUtdoor Droplets (CLOUD) chamber experiments proposed that in cold urban atmospheres with highly supersaturated HNO 3 and NH 3 , newly formed sub-10 nm nanoparticles can grow rapidly (up to 1000 nm h –1 ). Here, we present direct observational evidence that in winter Beijing with persistent highly supersaturated HNO 3 and NH 3 , nitrate contributed less than ~14% of the 8–40 nm nanoparticle composition, and overall growth rates were only ~0.8–5 nm h –1 . To explain the observed growth rates and particulate nitrate fraction, the effective mass accommodation coefficient of HNO 3 (α HNO 3 ) on the nanoparticles in urban Beijing needs to be 2–4 orders of magnitude lower than those in the CLOUD chamber. We propose that the inefficient uptake of HNO 3 on nanoparticles is mainly due to the much higher particulate organic fraction and lower relative humidity in urban Beijing. To quantitatively reproduce the observed growth, we show that an inhomogeneous “inorganic core–organic shell” nanoparticle morphology might exist for nanoparticles in Beijing. Finally, this study emphasized that growth for nanoparticles down to sub-10 nm was largely influenced by their composition, which was previously ignored and should be considered in future studies on nanoparticle growth.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1989

Observations and numerical simulations of precipitation development is seeded clouds over the Sierra Nevada

The evolution of precipitation in seeded wintertime orographically induced convective and stratiform clouds with embedded convection were studied using in situ observations and particle growth and trajectory models. The particle growth model of Heymsfield embedded in a kinematic flow field representative of the Sierra barrier was used to study the ice particle growth by diffusion, accretion and subsequent fall trajectories. The particles observed by the aircraft were classified into habits. The growth of observed particles were compared with the model predicted evolution. Using the aggregation model of Heymsfield, the observation of formation of aggregates is less than 10 minutes was verified. The key findings of this study are presented.

Prasad, N.↗
DOE OSTI2020

Large contribution of organics to condensational growth and formation of cloud condensation nuclei (CCN) in the remote marine boundary layer

Marine low clouds strongly influence global climate, and their radiative effects are particularly susceptible to the concentration of cloud condensation nuclei (CCN). One major source of CCN is the condensational growth of pre-CCN particles, and sulfate has long been considered the major condensing species in the remote marine boundary layer. While some studies have suggested that secondary organic species can contribute to particle growth, its importance remains unclear. Here we present the first long-term observational evidence that organics play an important role in particle growth over remote oceans. To the contrary of traditional thinking, sulfate dominated condensational growth for only a small (~18 %) fraction of the 62 observed growth events, even fewer than the organic-dominated events (24 %). During most (58 %) growth events, the major condensing species included both organics and sulfate. Potential precursors of the secondary organics are volatile organic compounds from ocean biological activities and those produced by the air–sea interfacial oxidation. Our results indicate that the condensation of secondary organics contributes strongly to the growth of pre-CCN particles and thereby the CCN population over remote oceans.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Hygroscopic Growth of UO 2 F 2 Particles

Hygroscopicity is an important physicochemical property of aerosol that describes the ability of a particle to uptake water. The hygroscopic properties of uranyl fluoride (UO 2 F 2 ) aerosol generated from a UF 6 hydrolysis reactor was investigated for the first time using a custom-built Humidified Tandem Differential Mobility Analyzer (HTDMA). The HTDMA is capable of measuring UO 2 F 2 particle growth determined by mobility size over a wide range of atmospheric humidity from dry conditions at <10% relative humidity (RH) to 85% RH. The hygroscopic properties were determined for nanoparticles as small as 3.5 nm in this study. Anhydrous UO 2 F 2 particles with a mobility diameter of 3.5 nm were shown to be highly hygroscopic with a deliquescence relative humidity (DRH) of 10%. Hydrates with a larger mobility diameter of 10 to 80 nm were non-hygroscopic with no observable DRH and limited water uptake up to 85% RH. These results demonstrate the hygroscopic properties of UO 2 F 2 particles are highly variable and based on both the mobility size and hydration state. Hygroscopicity affects the physicochemical properties of UO 2 F 2 particles, including the aerosol phase state and viscosity, with impacts on aerosol growth, coagulation, and deposition that is critical for understanding the fate and transport of UO 2 F 2 particles in the atmosphere.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1997

Characterization of Aircraft Produced Soot and Contrails Near the Tropopause

Participation in the SUCCESS project primarily involved development and deployment of specific instruments for characterizing jet aircraft exhaust emissions as particulates and their subsequent evolution as contrail particles, either liquid or solid, as cirrus. Observations can be conveniently considered in two categories - close or distant from the aircraft. Thus close to the aircraft the exhaust is mixing through the engine turbulence with a much drier and colder environment and developing water/ ice supersaturation along the trail depending on circumstances (near field), whereas distant from the aircraft (far field) the exhaust has cooled essentially to ambient temperature, the turbulence has decayed and any particle growth or evaporation is controlled by the prevailing ambient conditions. Intermediate between these two regions the main aircraft vortices form (one on each side of the aircraft) which tend to inhibit mixing under some conditions, a region extending from a few aircraft lengths to sometimes a hundred times this distance. Our approach to the problem lay in experience gained in characterizing the smoke from hydrocarbon combustion in terms of its cloud forming properties and its potential influence on the radiation properties of the smoke and subsequent cloud from the viewpoint of reduction (absorbtion and scattering ) of solar radiation flux leading to significant global cooling (Hudson et al 1991; Hallett and Hudson 1991). Engine exhaust contains a much smaller proportion of the fuel carbon than is sometimes present in ordinary combustion (less than 0.01% compared with 10%) and influences condensation in quite different ways, to be characterized by the Cloud Condensation Nucleus, CCN - supersaturation spectrum. The transition to ice is to be related to the dilution of solution droplets to freeze by homogeneous nucleation at temperatures somewhat below -40C (Pueschel et al 1998). The subsequent growth of ice particles depends critically on temperature, supersaturation and to some extent pressure, as is demonstrated in an NSF funded project being carried out in parallel with the work reported here. As will be discussed below, nucleation processes themselves and also exhaust impurities also influence the growth of ice particles and may control some aspects of growth of ice in contrails. Instrumentation was designed to give insight into these questions and to be flown on the NASA DC- 8 as a platform. In addition a modest program was undertaken to investigate the properties of laboratory produced smoke produced under controlled conditions from the viewpoint of forming both CCN and CN. The composition of the smoke could inferred from a thermal characterization technique; larger particles were captured by formvar replicator for detailed analysis; ice particles were captured and evaporated in flight on a new instrument, the cloudscope, to give their mass, density and impurity content.

Hallett, John↗
DOE OSTI2025

A radar view of ice microphysics and turbulence in Arctic cloud systems

Ice microphysical processes are inherently complex because of their sensitivity to temperature and humidity, the diversity of ice crystal habits, and their interaction with supercooled liquid water (SCL) and turbulence. Long-term surface-based radar observations have been systematically used to unravel the different processes that affect ice particle growth. In this study, we present a statistical analysis of 6.5 years of Ka-band radar observations in Arctic cloud systems, combined with thermodynamic profiles derived from radiosonde measurements. For the first time, ice particle growth and sublimation – diagnosed from vertical gradients of radar reflectivity and mean Doppler velocity – are systematically mapped across a broad range of temperature and moisture conditions. These vertical gradients correspond closely to saturation levels relative to ice and exhibit a strong temperature dependence in supersaturated regions. Notably, distinct signatures near −15 °C are indicative of dendritic growth. Turbulence, quantified via the eddy dissipation rate (EDR), is most frequently observed in regions containing SCL. The co-occurrence of SCL and elevated turbulence results in significantly enhanced ice particle growth compared to conditions in which either is present alone. This work provides new observational constraints that are critical for improving the representation of ice microphysics in atmospheric models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Computational fluid dynamics modeling and analysis of silica nanoparticle synthesis in a flame spray pyrolysis reactor

Flame Spray Pyrolysis (FSP) is a method for large-scale production of nanoparticles and nanoscale powders employed in a wide range of industrial applications. Particle size and morphology are complex functions of the physicochemical phenomena occurring in the FSP reactor. An extensive study of FSP-related phenomena can be utilized to develop effective strategies for achieving desired particle size/morphology and scaling up the overall yield of an FSP system. In this work, a computational fluid dynamics (CFD) model of an FSP reactor is developed to simulate the coupling of key phenomena involved in the particle synthesis process: liquid spray breakup and evaporation, mixing, combustion, and particle formation/growth of silica nanoparticles. Herein, the particle sizes and their distributions from the CFD simulations are validated against experimental data. Subsequently, the simulations are utilized to investigate the impact of process parameters on the resultant flame dynamics and particle growth. Firstly, the CFD results show that the particle sizes are strongly correlated with the precursor concentration in the solvent. At lower precursor concentrations, the spread of the distribution is relatively insensitive to the value of the concentration. At higher concentrations, the spread is higher as the collision probability between particles is higher. Secondly, increasing the pilot flow rate increases the length of the pilot flames impacting the local ignition location of the spray flame. Lastly, it is shown that the dispersion gas flow rate strongly influences the spray flame shape. This shape can be used for control of particle growth as it helps determine the regions of high temperature and the residence time of the particles in the high temperature region enabling the design and process optimization of the FSP reactor.

42 ENGINEERING↗
NASA NTRS2023

Can the Streaming Instability Form the First Planetesimals in Globally Turbulent Protoplanetary Disks?

Understanding the formation of the first planetesimals remains key to deciphering the history of planet formation within our own solar system and beyond. Evidence from the vast meteorite record [e.g., 1] as well as observations [e.g., 2] strongly suggest that the first planetesimals, and perhaps giant planet core accretion occurred well within the first million years of disk evolution. Moreover, chemical and lithological mixing as well as observations of line-broadening in protoplanetary disks (PPDs) [e.g., 3-6] suggest that the solar system nebula in this epoch was weakly-to-moderately turbulent in the regions where particle growth is of the greatest interest [7-8]. It is a well-known though that global hydrodynamic turbulence complicates particle growth due to a slew of barriers that can slow or even stall particle or aggregate growth at pebble sizes (with corresponding small particle Stokes numbers St) that can lead to loss to the central star via radial drift before planetesimals can ever form [9,10], requiring that some other mechanism come into play that collects growth-frustrated pebbles into gravitationally bound multi-km bodies – objects that are “born big” [11]. The current leading candidate for such a “leap-frog” mechanism is the so-called Streaming Instability (SI), a gas-drag mediated momentum exchange resonance in which the relative velocity between the particle component and a rotating gaseous fluid can lead to high densities in the particle field [12], which has been invoked in a number of recent PPD models that include a turbulent intensity α [e.g., 13-14] as the defacto mechanism for planetesimal formation if conditions for the SI (depending on particle St and the solids-to-gas mass ratio) are satisfied. However, these previous works use conditions established from occurrence studies for the onset of SI in laminar disks [15-17] in which the only source of turbulence is that self-generated by the settling particle layer, and not externally driven global turbulence. Recent analytical theories of the SI subject to global turbulence predict much more stringent conditions for the effectiveness of the SI than the laminar case [18-19]. Thus, whether the efficient operation of the SI can be attained in realistic models of the solar nebula have yet to be established. In this work, we ask whether the conditions under which the SI can produce gravitationally bound particle overdensities can actually be met in the first million years of evolution in globally turbulent PPDs.

P R Estrada↗
DOE OSTI2020

A Garnet-Type Solid-Electrolyte-Based Molten Lithium–Molybdenum–Iron(II) Chloride Battery with Advanced Reaction Mechanism

Solid-electrolyte-based molten-metal batteries have attracted considerable attention for grid-scale energy storage. Although ZEBRA batteries are considered one of the promising candidates, they still have the potential concern of metal particle growth and ion exchange with the β”-Al 2 O 3 electrolyte. Herein, a Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 solid-electrolyte-based molten lithium–molybdenum–iron(II) chloride battery (denoted as Li–Mo–FeCl 2 ) operated at temperature of 250 °C, comprising a mixture of Fe and LiCl cathode materials, a Li anode, a garnet-type Li-ion ceramic electrolyte, and Mo additive, is designed to overcome these obstacles. Different from conventional battery reaction mechanisms, this battery revolutionarily synchronizes the reversible Fe–Mo alloying–dealloying reactions with the delithiation–lithiation processes, meaning that the porous Mo framework derived from Fe–Mo alloy simultaneously suppresses the growth of pure Fe particles. By adopting a Li anode and a Li-ion ceramic electrolyte, the corrosion problem between the cathode and the solid electrolyte is overcome. With similar battery cost ($12 kWh –1 ), the theoretical energy density of Li–Mo–FeCl 2 battery surpasses that of a Na–FeCl 2 ZEBRA battery over 25%, to 576 Wh kg –1 and 2216 Wh L –1 , respectively. Experimental results further prove this cell has excellent cycling performance (472 mAh g LiCl –1 after 300 cycles, 50 mg active material) and strong tolerance against the overcharge–overdischarge (3–1.6 V) and freezing–thawing (25–250 °C) incidents.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Summer Aerosol and Trace Gas Observations in Houston, Texas Using an Adaptable Mobile Facility

An aerosol container featuring a shared inlet system was deployed to Houston, Texas in July 2022, enabling direct, high-time-resolution in situ measurements of aerosols and trace gases. The internal rack system and floorplan was designed for adaptable modularity to elucidate aerosol physicochemical processes at fine scales. The design allowed for the deployment of a core instrument suite and additional customized research grade instruments. A heterogeneous mixture of aerosols was observed during three regimes: (1) intermittent black carbon (BC) and diurnal variations in aerosol chemical composition, (2) observed particle growth associated with SO 2 , (3) transported supermicron dust. The high variability of observed particles and gases in high time resolution indicated a complex urban area with multiple local and regional sources and processes. Particle growth rates of 7–16 nm/hr were observed for submicron particles during periods when SO 2 was >0.5 ppbv. Two periods of multi-day long-range transport events of dust from the African Sahara were observed in the supermicron and submicron particle modes with total mass concentrations up to 30 μg m −3 . Aerosol scattering angstrom exponents and extinction coefficients (B ext ) increased with humidity as a function of particle composition. The measurements demonstrate collaborative capabilities that can be used to increase observations of aerosol processing, microphysical and optical properties, internal mixing state, and supermicron aerosol that are not parameterized or missing in global Earth energy system models.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1985

Studies of Model Immiscible Systems

The objectives are to use model transparent monotectics to obtain fundamental information applicable to two-phase systems in general, to apply this understanding to materials of interest in the Microgravity Science and Applications program, and to interpret results of flight experimental involving monotectic alloys. A number of model immiscible systems are in use to study various aspects of two-phase behavior within the miscibility gap and during solidification. Particle growth, coalescence and particle motions are under investigation using a holographic microscopy system. The system is capable of working with particle densities up to 10 to the 7th power particles/cubic centimeters through a 100 micron depth and can resolve particles of the order of 2 to 3 micron in diameter throughout the entire cell volume. Particle size, distribution changes with respect to time and temperature are observable from sequential holograms. Initial experiments using diethylene glycol/ethyl salicylate (DEG/ES) have demonstrated the usefulness of the technique. The thermal system controls temperature to at least plus or minus 0.001 K over the course of an experiment. A time-lapse film, made from holograms, of a succinonitrile/water solution shows particle size and number distribution changes with time under isothermal conditions. The observations are consistent with Ostwald ripening theory.

Frazier, D. O.↗
DOE OSTI2021

Aerodynamic effects on outer ash deposition rates in second generation atmospheric pressure oxy-coal combustion systems

Recent measurements in scenarios representative of second generation atmospheric pressure oxy-coal combustion systems have shown a significant increase in ash deposition rates in comparison to combustion in air. However, the causative mechanisms behind this increase have not been well understood. To fill this void, well-characterized experiments including fuel and deposit particle size distributions (PSDs) were coupled with highly resolved numerical simulations to isolate the aerodynamic effects impacting the deposition process such that mechanisms could be hypothesized. Three combustion scenarios (AIR, OXY27, OXY70) spanning a factor of three variation in flue gas volumetric flow rates were simulated and the deposition characteristics (impaction rates, deposit PSD, temperature, residence times, capture rates) tracked/predicted using a customized deposition module. The measured deposit PSD was significantly different from the PSD of the parent fuel indicating significant physio-chemical transformations (coalescence and particle growth in particular) at play. The use of simplistic modeling approaches (swelling parameter variations) to model particle growth led to inaccurate deposit ash PSD and rate predictions. A more satisfactory agreement between the measurements and simulations was obtained when the functional form of the parent fuel PSD (spread parameter) was modified to conform closely to the deposit PSD while still ensuring the fidelity of temperature and velocity predictions. Based on the measured ash compositions, identical capture criteria were employed across all three scenarios. Here this study further supports the theory that the ash deposition rates in these systems are dominated by aerodynamic effects with the ash PSD playing a dominant role.

42 ENGINEERING↗
DOE OSTI2022

Rapid growth of anthropogenic organic nanoparticles greatly alters cloud life cycle in the Amazon rainforest

Aerosol-cloud interactions remain uncertain in assessing climate change. While anthropogenic activities produce copious aerosol nanoparticles smaller than 10 nanometers, they are too small to act as efficient cloud condensation nuclei (CCN). The mechanisms responsible for particle growth to CCN-relevant sizes are poorly understood. Here, we present aircraft observations of rapid growth of anthropogenic nanoparticles downwind of an isolated metropolis in the Amazon rainforest. Model analysis reveals that the sustained particle growth to CCN sizes is predominantly caused by particle-phase diffusion-limited partitioning of semivolatile oxidation products of biogenic hydrocarbons. Cloud-resolving numerical simulations show that the enhanced CCN concentrations in the urban plume substantially alter the formation of shallow convective clouds, suppress precipitation, and enhance the transition to deep convective clouds. The proposed nanoparticle growth mechanism, expressly enabled by the abundantly formed semivolatile organics, suggests an appreciable impact of anthropogenic aerosols on cloud life cycle in previously unpolluted forests of the world.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2001

Mechanistic Studies of Combustion and Structure Formation During Synthesis of Advanced Materials

Combustion in a variety of heterogeneous systems, leading to the synthesis of advanced materials, is characterized by high temperatures (2000-3500 K) and heating rates (up to 10(exp 6) K/s) at and ahead of the reaction front. These high temperatures generate liquids and gases which are subject to gravity-driven flow. The removal of such gravitational effects is likely to provide increased control of the reaction front, with a consequent improvement in control of the microstructure of the synthesized products. Thus, microgravity (mu-g) experiments lead to major advances in the understanding of fundamental aspects of combustion and structure formation under the extreme conditions of the combustion synthesis (CS) wave. In addition, the specific features of microgravity environment allow one to produce unique materials, which cannot be obtained under terrestrial conditions. The current research is a logic continuation of our previous work on investigations of the fundamental phenomena of combustion and structure formation that occur at the high temperatures achieved in a CS wave. Our research is being conducted in three main directions: 1) Microstructural Transformations during Combustion Synthesis of Metal-Ceramic Composites. The studies are devoted to the investigation of particle growth during CS of intermetallic-ceramic composites, synthesized from nickel, aluminum, titanium, and boron metal reactants. To determine the mechanisms of particle growth, the investigation varies the relative amount of components in the initial mixture to yield combustion wave products with different ratios of solid and liquid phases, under 1g and mu-g conditions; 2) Mechanisms of Heat Transfer during Reactions in Heterogeneous Media. Specifically, new phenomena of gasless combustion wave propagation in heterogeneous media with porosity higher than that achievable in normal gravity conditions, are being studied. Two types of mixtures are investigated: clad powders, where contact between reactants occurs within each particle, and mixtures of elemental powders, where interparticle contacts are important for the reaction; and 3) Mechanistic Studies of Phase Separation in Combustion of Thermite Systems. Studies are devoted to experiments on thermite systems (metal oxide-reducing metal) where phase separation processes occur to produce alloys with tailored compositions and properties. The separation may be either gravity-driven or due to surface forces, and systematic studies to elucidate the true mechanism are being conducted. The knowledge obtained will be used to find the most promising ways of controlling the microstructure and properties of combustion-synthesized materials. Low-gravity experiments are essential to create idealized an environment for insights into the physics and chemistry of advanced material synthesis processes.

Varma, A.↗
NASA NTRS1998

Turbulent Radiation Effects in HSCT Combustor Rich Zone

A joint UTRC-University of Connecticut theoretical program was based on describing coupled soot formation and radiation in turbulent flows using stretched flamelet theory. This effort was involved with using the model jet fuel kinetics mechanism to predict soot growth in flamelets at elevated pressure, to incorporate an efficient model for turbulent thermal radiation into a discrete transfer radiation code, and to couple die soot growth, flowfield, and radiation algorithm. The soot calculations used a recently developed opposed jet code which couples the dynamical equations of size-class dependent particle growth with complex chemistry. Several of the tasks represent technical firsts; among these are the prediction of soot from a detailed jet fuel kinetics mechanism, the inclusion of pressure effects in the soot particle growth equations, and the inclusion of the efficient turbulent radiation algorithm in a combustor code.

Hall, Robert J.↗
NASA NTRS1994

Coagulation of grains in static and collapsing protostellar clouds

We simulate collisional evolution of grains in dense turbulent molecular cloud cores (or Bok globules) in static equilibrium and free-fall collapse, assuming spherical symmetry. Relative velocities are due to thermal motions, differential settling, and turbulence, with the latter dominant for sonic turbulence with an assumed Kolmogorov spectrum. Realistic criteria are used to determine outcomes of collisions (coagulation vs. destruction) as functions of particle size and velocity. Results are presented for a variety of cloud parameters (radial density profile, turbulent velocity) and particle properties (density, impact strength). Results are sensitive to the assumed mechanical properties (density and impact strength) of grain aggregates. Particle growth is enhanced if aggregates have low density or fractal structures. On a timescale of a few Myr, an initial population of 0.1 micrometers grains may produce dense compact particles approximately 1 micrometer in size, or fluffy aggregates approximately 100 micrometers. For impact strengths less than or equal to 10(exp 6) ergs/g, a steady state is reached between coagulation of small grains and collisional disruption of larger aggregates. Formation of macroscopic aggregates requires high mechanical strengths and low aggregate densities. We assume sonic turbulence during collapse, with varied eddy size scales determining the dissipation rate or turbulence strength. The degree of collisional evolution during collapse is sensitive to the assumed small-scale structure (inner sc ale) of the turbulence. Weak turbulence results in few collisions and preserves the precollapse particle size distribution with little change. Strong turbulence tends to produce net destruction, rather than particle growth, during infall, unless inpact strengths are greater than 10(exp 6)ergs/g.

Weidenschilling, S. J.↗
DOE OSTI2023

Substantially positive contributions of new particle formation to cloud condensation nuclei under low supersaturation in China based on numerical model improvements

New particle formation (NPF) and subsequent particle growth are important sources of condensation nuclei (CN) and cloud condensation nuclei (CCN). While many observations have shown positive contributions of NPF to CCN at low supersaturation, negative NPF contributions were often simulated in polluted environments. Using the observations in a coastal city of Qingdao, Beijing, and Gucheng in north China, we thoroughly evaluate the simulated number concentrations of CN and CCN using an NPF-explicit parameterization embedded in the WRF-Chem model. For CN, the initial simulation shows large biases of particle number concentrations at 10–40 and 40–100 nm. By adjusting the process of gas–particle partitioning, including the mass accommodation coefficient (MAC) of sulfuric acid, the phase changes in primary organic aerosol emissions, and the condensational amount of nitric acid, the improvement of the particle growth process yields substantially reduced overestimation of CN. Regarding CCN, secondary organic aerosol (SOA) formed from the oxidation of semi-volatile and intermediate-volatility organic compounds (S/IVOCs) is called SI-SOA, the yield of which is an important contributor. At default settings, the SI-SOA yield is too high without considering the differences in precursor oxidation rates. Lowering the SI-SOA yield under linear H 2 SO 4 nucleation scheme results in much-improved CCN simulations compared to observations. On the basis of the bias-corrected model, we find substantially positive contributions of NPF to CCN at low supersaturation (~ 0.2 %) over broad areas of China, primarily due to competing effects of increasing particle hygroscopicity, a result of reductions in SI-SOA amount, surpassing that of particle size decreases. The bias-corrected model is robustly applicable to other schemes, such as the quadratic H 2 SO 4 nucleation scheme, in terms of CN and CCN, though the dependence of CCN on SI-SOA yield is diminished likely due to changes in particle composition. This study highlights potentially much larger NPF contributions to CCN on a regional and even global basis.

54 ENVIRONMENTAL SCIENCES↗