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At least 55 records · Page 3

Thermophysical modeling of raw glaze liquidus temperature and viscosity

Raw glazes, which do not contain pre-melted glass frits, are widely used due to their low cost. The natural variability of the mineral compositions used in raw glazes affects their viscosity during firing. Molten glaze viscosity plays an important role in determining the final surface quality; therefore, it is important to determine how raw glaze composition and firing conditions affect viscosity. Thermophysical modeling provides a way to evaluate the liquidus temperature and viscosity of molten glazes as a function of composition and oxygen activity. Equilibrium phase volume fraction and composition of 242 raw glaze recipes were evaluated under oxidizing and reducing conditions. Undissolved or precipitation of solid phases explain the secondary flux transition from anti-fluxing to fluxing near the liquidus temperature. The liquidus temperature and viscosity of iron glazes decrease as a function of increasing iron content under a reducing atmosphere. The empirical probability distribution of molten glaze viscosity follows a lognormal distribution, with lead glazes having significantly lower viscosity compared with glazes without lead. Here, the peak firing temperature viscosity of lead-free glazes is near the working point of glass. Multiple linear regression analysis shows that the peak firing temperature viscosity and liquidus temperature significantly predict the viscosity factor.

36 MATERIALS SCIENCE↗

Universal Solvent Viscosity Reduction via Hydrogen Bonding Disruptors

Liquid Ion Solutions LLC (DBA RoCo Global) in partnership with Carnegie Mellon University and Carbon Capture Scientific LLC, has performed lab-scale development and evaluation of novel additives that lower the viscosity of water-lean amine solvents for post-combustion carbon dioxide capture. This project focuses on developing additives that minimize the formation of long-range electrostatic and hydrogen bonding (HB) networks, decreasing the solvent viscosity, improving diffusion, and improving the process economics. The project objectives included: 1) performing computer simulation to understand the molecular interactions of the additive molecules in water-lean CO 2 capture solvents, 2) design and synthesis of HB disruptors additives, 3) performance testing with additive molecules on model amine solvents, and 4) demonstration of the effectiveness of the optimized additives in the presence of synthetic flue gas. To meet the abovementioned objectives, the project team utilized a holistic approach that combines molecular simulation, experimental testing, and economic analysis studies. The project team developed ab initio molecular model and then perform computer simulation to develop relationship between hydrogen bonding, viscosity, and performed quantitative analysis of additive on the viscosity of the solvent. The team completed computational comparative study on a range of organic functional groups such as ethers, esters, cyclic carbonates, alkanes, and ammonium salts for their effect on viscosity gaining key insights into molecular interactions and the impact of various functional groups and molecular shapes on viscosity. Assisted with molecular simulation insights, the project team conducted additive synthesis and testing, including a proof-of-concept study, additive screening, optimization, and synthetic flue gas testing. The experimental proof-of-concept study proved that the hydrogen bonding acceptors result in significant decrease of viscosities. Detailed additive screening (exploring various functionalities and molecular structures) has been performed. Several promising additives showed excellent reduction in viscosity (30-41%) at 5% additive loading, and over 50% viscosity reduction at 10% additive loading for the model solvents. The team also performed complex screening studies on additive loadings and mixing effect among additives using the design of experiments. Based on multiple screening experiments, one additive-solvent candidate was down-selected for synthetic flue gas testing. A 100-hour continuous absorption/desorption study was conducted under simulated flue gas using a lab-scale continuous capture and separation system. No degradation (for both solvent and additive) was observed based on the GC results of the solvent samples collected from the continuous study. The team conducted preliminary engineering analyses and cost-benefit analyses to quantify the potential economic benefits of the additive approach for solvent viscosity reduction. Based on the experimental data, CO 2 capture cost savings from the capital and operating cost savings are estimated at $\$$4.7/tonne and $\$$0.3/tonne CO 2 captured, respectively. Considering the additive cost, the net benefit is estimated to be between $\$$4.32~$\$$4.86/tonne CO 2 captured.

20 FOSSIL-FUELED POWER PLANTS↗

Reduced viscosity steadily weakens oceanic currents

The viscosity of both air and water is temperature dependent. A rising temperature leads to an increased viscosity for air but a decreased viscosity for water. As climate becomes warmer, this increased air viscosity can partly inhibit the reduction of wind stress over the ocean, and the reduced water viscosity causes less downward momentum and heat transport. As these opposing effects of warming on air and water viscosity are not included in the state-of-the-art climate models, the understanding of their potential impacts on the response of the climate system to the anthropogenic warming is lacking. Here, via analyzing the Simple Ocean Data Assimilation oceanic reanalysis dataset, we show that the ocean heat content increases at a rate of ~1.3 × 10 22 J/yr over 35 years, which leads to a continuous reduction of oceanic viscosity. As a result, the ocean vertical shear enhances with a shoaling of the mixed layer depth and a reduced vertical linkage in the ocean. Our calculations show a reduction of the oceanic kinetic energy at a rate of ~2.4 × 10 16 J/yr. Potentially, this could generate far-reaching impacts on the energy storage of the climate system and, hence, could pace the global warming. Thus, it is important to include the temperature-dependent viscosity in our climate models. Freshwater discharged from polar ice sheets and mountain glaciers also contributes to the reduction in oceanic viscosity but, at present, to a lesser extent than that in oceanic warming. Reduced oceanic viscosity, therefore, is an important, but hitherto overlooked, response to a warming climate and contributes to many recent weather extremes including heavier rainfall rates in hurricanes, slackening of the polar vortex, and oceanic heat waves.

54 ENVIRONMENTAL SCIENCES↗

Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition

Secondary organic aerosol (SOA) accounts for a large fraction of submicron particles in the atmosphere. SOA can occur in amorphous solid or semi-solid phase states depending on chemical composition, relative humidity (RH), and temperature. The phase transition between amorphous solid and semi-solid states occurs at the glass transition temperature ( T g ). We have recently developed a method to estimate T g of pure compounds containing carbon, hydrogen, and oxygen atoms (CHO compounds) with molar mass less than 450 g mol -1 based on their molar mass and atomic O : C ratio. In this study, we refine and extend this method for CH and CHO compounds with molar mass up to ~1100 g mol -1 using the number of carbon, hydrogen, and oxygen atoms. We predict viscosity from the T g -scaled Arrhenius plot of fragility (viscosity vs. T g / T ) as a function of the fragility parameter D . We compiled D values of organic compounds from the literature and found that D approaches a lower limit of ~10 (±1.7) as the molar mass increases. We estimated the viscosity of α -pinene and isoprene SOA as a function of RH by accounting for the hygroscopic growth of SOA and applying the Gordon–Taylor mixing rule, reproducing previously published experimental measurements very well. Sensitivity studies were conducted to evaluate impacts of T g , D , the hygroscopicity parameter ( κ ), and the Gordon–Taylor constant on viscosity predictions. The viscosity of toluene SOA was predicted using the elemental composition obtained by high-resolution mass spectrometry (HRMS), resulting in a good agreement with the measured viscosity. We also estimated the viscosity of biomass burning particles using the chemical composition measured by HRMS with two different ionization techniques: electrospray ionization (ESI) and atmospheric pressure photoionization (APPI). Due to differences in detected organic compounds and signal intensity, predicted viscosities at low RH based on ESI and APPI measurements differ by 2–5 orders of magnitude. Complementary measurements of viscosity and chemical composition are desired to further constrain RH-dependent viscosity in future studies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DWPF STARTUP FRIT VISCOSITY MEASUREMENT ROUND ROBIN RESULTS

A viscosity standard is needed to replace the National Institute of Standards and Technology (NIST) glasses currently being used to calibrate viscosity measurement equipment. The current NIST glasses are either unavailable or less than ideal for calibrating equipment to measure the viscosity of high-level waste glasses. This report documents the results of a viscosity round robin study conducted on the Defense Waste Processing Facility (DWPF) startup frit. DWPF startup frit was selected because its viscosity-temperature relationship is similar to most DWPF and Hanford high-level waste glass compositions. The glass underwent grinding and blending to homogenize the large (100 lb) batch. Portions of the batch were supplied to the laboratories (named A through H) for viscosity measurements following a specified temperature schedule with a temperature range of 1150 C to 950 C and with an option to measure viscosity at lower temperatures if their equipment was capable of measuring at the higher viscosities. Results were used to fit the Vogel-Tamman-Fulcher and Arrhenius equations to viscosity as a function of temperature for the entire temperature range of 460 C through 1250 C as well as the limited temperature interval of approximately 950 C through 1250 C. The standard errors for confidence and prediction were determined for the fitted models.

36 MATERIALS SCIENCE↗

Measurements and Model Estimations of Viscosities of the MnO-CaO-SiO{sub 2}-MgO-Al{sub 2}O{sub 3} Melts

The viscosities of the MnO (0 to 55 mass pct)-CaO-SiO{sub 2}-MgO (5 mass pct)-Al{sub 2}O{sub 3} (20 mass pct) melts were measured by rotating cylinder method in the temperature range from 1573 K to 1873 K (1300 °C to 1600 °C). The measurements were carried out in the atmosphere of flowing CO/CO{sub 2} gas mixture with a volume ratio of 99/1, and molybdenum crucible and spindle were adopted. The results reveal that MnO is a viscosity reducing component, and the effect of MnO is more notable in the melts with higher ratio of CaO to SiO{sub 2}. For example, in the melts with the mass ratio of CaO to SiO{sub 2} equal to 0.6, the addition of 5 mass pct MnO only slightly reduced the viscosities. Comparatively, the addition of 5 mass pct MnO made the viscosities of the melts with the mass ratio of CaO to SiO{sub 2} equal to 1.0 and 1.5 decrease remarkably. Based on the measured data, the viscosities estimation model proposed in our previous study was extended to the system containing MnO, and the model parameters were determined. The model can estimate and predict the viscosities of the aluminosilicate melts containing MnO well, and then some iso-viscosity contours of this system were calculated. From the iso-viscosity contours, it can be seen that MnO is almost equivalent to CaO in reducing the viscosities in the melt with high SiO{sub 2} content, while with the decrease of the SiO{sub 2} content MnO becomes more effective than CaO.

36 MATERIALS SCIENCE↗

The effect of artificial bulk viscosity in simulations of forced compressible turbulence

The use of an artificial bulk viscosity for shock stabilization is a common approach employed in turbulence simulations with high-order numerics. The effect of the artificial bulk viscosity is analyzed in the context of large eddy simulations by using as a test case simulations of linearly-forced compressible homogeneous turbulence (Petersen and Livescu, 2010 [12]). This case is unique in that it allows for the specification of a priori target values for total dissipation and ratio of solenoidal to dilatational dissipation. A comparison between these target values and the true predicted levels of dissipation is thus used to investigate the performance of the artificial bulk viscosity. Results show that the artificial bulk viscosity is effective at achieving stable solutions, but also leads to large values of artificial dissipation that outweigh the physical dissipation caused by fluid viscosity. An alternate approach, which employs the artificial thermal conductivity only, shows that the dissipation of dilatational modes is entirely due to the fluid viscosity. However, this method leads to unwanted Gibbs oscillations around the shocklets. The use of shock sensors that further localize the artificial bulk viscosity did not reduce the amount of artificial dissipation introduced by the artificial bulk viscosity. Finally, an improved forcing function that explicitly accounts for the role of the artificial bulk viscosity in the budget of turbulent kinetic energy was explored.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

THE EFFECT OF ANISOTROPIC VISCOSITY ON COLD FRONTS IN GALAXY CLUSTERS

Cold fronts—contact discontinuities in the intracluster medium (ICM) of galaxy clusters—should be disrupted by Kelvin-Helmholtz (K-H) instabilities due to the associated shear velocity. However, many observed cold fronts appear stable. This opens the possibility of placing constraints on microphysical mechanisms that stabilize them, such as the ICM viscosity and/or magnetic fields. We performed exploratory high-resolution simulations of cold fronts arising from subsonic gas sloshing in cluster cores using the grid-based Athena MHD code, comparing the effects of isotropic Spitzer and anisotropic Braginskii viscosity (expected in a magnetized plasma). Magnetized simulations with full Braginskii viscosity or isotropic Spitzer viscosity reduced by a factor f ∼ 0.1 are both in qualitative agreement with observations in terms of suppressing K-H instabilities. The rms velocity of turbulence within the sloshing region is only modestly reduced by Braginskii viscosity. We also performed unmagnetized simulations with and without viscosity and find that magnetic fields have a substantial effect on the appearance of the cold fronts, even if the initial field is weak and the viscosity is the same. This suggests that determining the dominant suppression mechanism of a given cold front from X-ray observations (e.g., viscosity or magnetic fields) by comparison with simulations is not straightforward. Finally, we performed simulations including anisotropic thermal conduction, and find that including Braginskii viscosity in these simulations does not significantly affect the evolution of cold fronts; they are rapidly smeared out by thermal conduction, as in the inviscid case.

79 ASTRONOMY AND ASTROPHYSICS↗

Predicted viscosity of liquid HMX up to 40 GPa

Viscous flow serves as a significant heating mechanism during the formation of hot spots, but the shear viscosity which determines this response is poorly characterized for most high explosives. Most recently, a model was proposed for the shear viscosity of liquid HMX (1,3,5,7-tetranitro-1,3,5,7-tetrazocane) that was fit to pressures reaching 5 GPa, but this work uncovered uncertainties in the viscosity at 0 GPa and remains untested at higher pressures. We use molecular dynamics (MD) simulations and the Green-Kubo formalism to predict the temperature- and pressure-dependent shear viscosity of HMX over the pressure interval 0 GPa≤P≤40 GPa. Reassessment of the viscosity at 0 GPa rules out several potential explanations for discrepancies between earlier reports; we attribute these differences to details of MD trajectory integration impacting molecular flexibility. The shear viscosity of HMX exhibits an Arrhenius temperature dependence at each pressure considered, with exponential prefactor and activation energy terms that are also strong functions of pressure. An analytic form for the viscosity is developed based on an extension of the well-known Andrade equation that simultaneously captures the temperature and pressure dependencies in the MD data up to 40 GPa. Comparison against a recently developed model for the viscosity of liquid RDX (1,3,5-trinitro-1,3,5-triazinane) shows that both materials exhibit similar functional dependencies with the viscosity of HMX being higher by roughly an order of magnitude at a given temperature-pressure state.

36 MATERIALS SCIENCE↗

Effect of surface viscosity, anchoring energy, and cell gap on the response time of nematic liquid crystals

An analytical expression for the relaxation time of a nematic liquid crystal is obtained for the first time by considering the influence of surface viscosity, anchoring energy strength and cell gap, validated numerically by using the so-called relaxation method. This general equation for the molecular response time (τ{sub 0}) was derived for a vertical aligned cell and by solving an eigenvalue equation coming from the usual balance of torque equation in the Derzhanskii and Petrov formulation, recovering the usual equations in the appropriate limit. The results show that τ∼d{sup b}, where b=2 is observed only for strongly anchored cells, while for moderate to weak anchored cells, the exponent lies between 1 and 2, depending on both, surface viscosity and anchoring strength. We found that the surface viscosity is important when calculating the response time, specially for thin cells, critical for liquid crystal devices. The surface viscosity’s effect on the optical response time with pretilt is also explored. Our results bring new insights about the role of surface viscosity and its effects in applied physics. - Highlights: • The relaxation of nematic liquid crystals is calculated by taking the surface viscosity into account. • An analytical expression for the relaxation time depending on surface viscosity, anchoring strength and cell gap is obtained. • The results are numerically verified. • Surface viscosity is crucial for thin and weak anchored cells. • The effect on optical time and pretilt angle is also studied.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Arrhenian to non-Arrhenian crossover in glass melt viscosity

The activation energy for glass melt viscosity is a function of temperature, i.e., non-Arrhenian, within a middle range of viscosity values (typically, between 10 2 and 10 10 Pa s) and constant, i.e., Arrhenian, outside this range. At the low-viscosity end, the Arrhenian to non-Arrhenian transition (termed the crossover) falls within the glass processing range: glass melting and fining occur within the Arrhenian range while glass forming occurs within the non-Arrhenian range. By the Adam-Gibbs equation, the configuration entropy is nearly constant at high temperatures (low viscosities), where the glass melt turns into a simple liquid, and decreases with decreasing temperature (increasing viscosity) as the glass is increasingly polymerized. In the present study, the power-law function and hyperbolic tangent function are used to express the configuration entropy as a function of temperature. The viscosity crossover is defined as the point at which onset of structural grouping is causing the configuration entropy to deviate from its high-temperature value. In conclusion, it appears that the limited range of the configuration entropy of the fully depolymerized melt imposes a restriction on the crossover viscosity; for well-defined glass families, such as float glasses or nuclear waste glasses, the crossover point can be defined using a fixed, i.e., composition-independent, viscosity value.

36 MATERIALS SCIENCE↗

Viscosity of 1-Alkyl-1-methylpyrrolidinium Bis(trifluoromethylsulfonyl)imide Ionic Liquids Saturated with Compressed CO 2

The viscosity of mixtures of pyrrolidinium-based ionic liquids saturated with compressed CO 2 was measured using a high-pressure viscometer at three different temperatures (298.15, 318.15 and 338.15 K). The high-pressure viscosity of 1-propyl-1-methyl-pyrrolidinium ([C 3 C 1 pyr]), 1-butyl-1-methyl-pyrrolidinium ([C 4 C 1 pyr]), and 1-hexyl-1-methyl-pyrrolidinium bis(trifluoromethylsulfonyl)amide ([C 6 C 1 pyr]) cations with common anion, bis(trifluoromethylsulfonyl)amide ([NTf 2 ]), was measured up to a maximum CO 2 pressure of 25 MPa. In the temperature range investigated, the viscosity of the ionic liquid/ CO 2 mixture dramatically decreases with increasing of CO 2 pressure up to approximately 7 MPa but the viscosity decrease becomes less significant at higher CO 2 pressures (from 7 to 25 MPa) because the CO 2 composition in ILs slightly increases with pressure. At lower CO 2 pressures (compositions), temperature has a higher impact on the CO 2 solubility in IL, thus the viscosity drops significantly for lower temperatures (e.g. 298.15 K). The effect of alkyl chain length of the cation on the viscosity of ionic liquid/ CO 2 mixture was also measured. Though the pure [C n C 1 pyr][NTf 2 ] viscosity increases significantly with the increasing alkyl chain length of the cation, the viscosity of every ionic liquid/ CO 2 mixture tested herein become quite similar at higher CO 2 pressures, for a fixed temperature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Note: Precision viscosity measurement using suspended microchannel resonators

We report the characterization of a suspended microchannel resonator (SMR) for viscosity measurements in a low viscosity regime (<10 mPa s) using two measurement schemes. First, the quality factor (Q-factor) of the SMR was characterized with glycerol-water mixtures. The measured Q-factor at 20 Degree-Sign C exhibits a bilinear behavior with the sensitivity of 1281 (mPa s){sup -1} for a lower (1-4 mPa s) and 355 (mPa s){sup -1} for a higher viscosity range (4-8 mPa s), respectively. The second scheme is the vibration amplitude monitoring of the SMR running in a closed loop feedback. When compared in terms of the measurement time, the amplitude-based measurement takes only 0.1 {approx} 1 ms while the Q-factor-based measurement takes {approx}30 s. However, the viscosity resolution of the Q-factor-based measurement is at least three times better than the amplitude-based measurement. By comparing the Q-factors of heavy water and 9.65 wt.% glycerol-water mixture that have very similar viscosities but different densities, we confirmed that the SMR can measure the dynamic viscosity without the density correction. The obtained results demonstrate that the SMR can measure the fluid viscosity with high precision and even real-time monitoring of the viscosity change is possible with the amplitude-based measurement scheme.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Intrinsic bulk viscosity of the one-component plasma

The intrinsic bulk viscosity of the one-component plasma (OCP) is computed and analyzed using equilibrium molecular dynamics simulations and the Green-Kubo formalism. It is found that bulk viscosity exhibits a maximum at Γ ≈ 1, corresponding to the condition that the average kinetic energy of particles equals the potential energy at the average interparticle spacing. The weakly coupled and strongly coupled limits are analyzed and used to construct a model that captures the full range of coupling strengths simulated: Γ ≈ 10 –2 –10 2 . Simulations are also run of the Yukawa one-component plasma (YOCP) in order to understand the impact of electron screening. It is found that electron screening leads to a smaller bulk viscosity due to a reduction in the excess heat capacity of the system. Bulk viscosity is shown to be at least an order of magnitude smaller than shear viscosity in both the OCP and YOCP. The generalized frequency-dependent bulk viscosity coefficient is also analyzed. This is found to exhibit a peak near twice the plasma frequency in strongly coupled conditions, which is associated with the oscillatory decay observed in the bulk viscosity autocorrelation function. As a result, the generalized shear and bulk viscosity coefficients are found to have a similar magnitude for ω ≳ 2⁢ω p at strongly coupled conditions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Error quantification of the Arrhenius blending rule for viscosity of hydrocarbon mixtures

Six hundred and seventy-five measurements of dynamic viscosity and density have been used to assess the prediction error of the Arrhenius blending rule for kinematic viscosity of hydrocarbon mixtures. Major trends within the data show that mixture complexity–binary to hundreds of components—and temperature are more important determinants of prediction error than differences in molecular size or hydrogen saturation between the components of the mixtures. Over the range evaluated, no correlation between prediction error and mole fractions was observed, suggesting the log of viscosity truly is linear in mole fraction, as indicated by the Arrhenius blending rule. Mixture complexity and temperature also impact molar volume and its prediction. However, a linear regression between the two model errors explains less than 20% of the observed variation, indicating that mixture viscosity and/or molar volume are not linear with respect to temperature and/or mixture complexity. Extensive discussion of the intermolecular forces and the geometric arrangement of molecules and vacancies in liquids, which ultimately determines its viscosity, is brought into context with the implicit approximations behind the Arrhenius blending rule. The complexity of this physics is not compatible with a simple algebraic correction to the model. However, sufficient data is now available to determine confidence intervals around the prediction of fuel viscosity based on its component mole fractions and viscosities. At -40°C, when all identified components are pure molecules the modeling error is 13.2% of the predicted (nominal) viscosity times the root mean square of the component mole fractions.

10 SYNTHETIC FUELS↗

Predicted Melt Curve and Liquid Shear Viscosity of RDX up to 30 GPa

Recent grain-scale simulations of HMX and TATB have shown that predictions for hot spot formation in high explosives are particularly sensitive to accurate determinations of the pressure-dependent melt curve and the shear viscosity of the liquid phase. These physics terms are poorly constrained beyond ambient pressure for the explosive RDX. Here we adopt an all-atom modeling approach using molecular dynamics (MD) simulations to predict the melt curve of RDX near to detonation conditions (30 GPa) and determine the shear viscosity of the liquid as a function of temperature and pressure above the melt curve. Phase-coexistence simulations were used to determine the melt curve, which is predicted to vary by almost 1100 K as the pressure increases from 0 GPa to 30 GPa. Equilibrium MD simulations and the Green-Kubo formalism were used to obtain the pressure-temperature-dependent shear viscosity. The shear viscosity of RDX is predicted to be of similar magnitude to the viscosity of TATB at low GPa-range pressures, and to be roughly an order of magnitude lower than the viscosity of HMX. The temperature dependence of the shear viscosity is Arrhenius at a given pressure, and the exponential pre-factor and activation term exhibit a strong, yet complicated, pressure dependence. An empirical pressure-temperature dependent function for RDX shear viscosity is developed that simultaneously captures a wide range of MD predictions while taking an analytic form that extrapolates smoothly beyond the fitted regime. The relative strength of the pressure and temperature dependencies of these two physics terms is found to be of similar magnitude for RDX, HMX, and TATB, which motivates incorporating these results in future RDX grain-scale modeling.

36 MATERIALS SCIENCE↗

Estimation of secondary organic aerosol viscosity from explicit modeling of gas-phase oxidation of isoprene and α -pinene

Abstract. Secondary organic aerosols (SOA) are major components of atmospheric fine particulate matter, affecting climate and air quality. Mounting evidence exists that SOA can adopt glassy and viscous semisolid states, impacting formation and partitioning of SOA. In this study, we apply the GECKO-A (Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere) model to conduct explicit chemical modeling of isoprene photooxidation and α-pinene ozonolysis and their subsequent SOA formation. The detailed gas-phase chemical schemes from GECKO-A are implemented into a box model and coupled to our recently developed glass transition temperature parameterizations, allowing us to predict SOA viscosity. The effects of chemical composition, relative humidity, mass loadings and mass accommodation on particle viscosity are investigated in comparison with measurements of SOA viscosity. The simulated viscosity of isoprene SOA agrees well with viscosity measurements as a function of relative humidity, while the model underestimates viscosity of α-pinene SOA by a few orders of magnitude. This difference may be due to missing processes in the model, including autoxidation and particle-phase reactions, leading to the formation of high-molar-mass compounds that would increase particle viscosity. Additional simulations imply that kinetic limitations of bulk diffusion and reduction in mass accommodation coefficient may play a role in enhancing particle viscosity by suppressing condensation of semi-volatile compounds. The developed model is a useful tool for analysis and investigation of the interplay among gas-phase reactions, particle chemical composition and SOA phase state.

54 ENVIRONMENTAL SCIENCES↗

Toward closure between predicted and observed particle viscosity over a wide range of temperatures and relative humidity

Abstract. Atmospheric aerosols can exist in amorphous semi-solid or glassy phase states whose viscosity varies with atmospheric temperature and relative humidity. The temperature and humidity dependence of viscosity has been hypothesized to be predictable from the combination of a water–organic binary mixing rule of the glass transition temperature, a glass-transition-temperature-scaled viscosity fragility parameterization, and a water uptake parameterization. This work presents a closure study between predicted and observed viscosity for sucrose and citric acid. Viscosity and glass transition temperature as a function of water content are compiled from literature data and used to constrain the fragility parameterization. New measurements characterizing viscosity of sub-100 nm particles using the dimer relaxation method are presented. These measurements extend the available data of temperature- and humidity-dependent viscosity to −28 ∘C. Predicted relationships agree well with observations at room temperature and with measured isopleths of constant viscosity at ∼107 Pa s at temperatures warmer than −28 ∘C. Discrepancies at colder temperatures are observed for sucrose particles. Simulations with the kinetic multi-layer model of gas–particle interactions suggest that the observed deviations at colder temperature for sucrose can be attributed to kinetic limitations associated with water uptake at the timescales of the dimer relaxation experiments. Using the available information, updated equilibrium phase-state diagrams (-80∘C

54 ENVIRONMENTAL SCIENCES↗