A thermodynamic framework for bulk–surface partitioning in finite-volume mixed organic–inorganic aerosol particles and cloud droplets

Atmospheric aerosol particles and their interactions with clouds are among the largest sources of uncertainty in global climate modeling. Aerosol particles in the ultrafine size range with diameters less than 100 nm have very high surface-area-to-volume ratios, with a substantial fraction of molecules occupying the air–droplet interface. The partitioning of surface-active species between the interior bulk of a droplet and the interface with the surrounding air plays a large role in the physicochemical properties of a particle and in the activation of ultrafine particles, especially those of less than 50 nm diameter, into cloud droplets. In this work, a novel and thermodynamically rigorous treatment of bulk–surface equilibrium partitioning is developed through the use of a framework based on the Aerosol Inorganic–Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model in combination with a finite-depth Guggenheim interface region on spherical, finite-volume droplets. We outline our numerical implementation of the resulting modified Butler equation, including accounting for challenging extreme cases when certain compounds have very limited solubility in either the surface or the bulk phase. This model, which uses a single, physically constrained interface thickness parameter, is capable of predicting the size-dependent surface tension of complex multicomponent solutions containing organic and inorganic species. We explore the impacts of coupled surface tension changes and changes in bulk–surface partitioning coefficients for aerosol particles ranging in diameters from several micrometers to as small as 10 nm and across atmospherically relevant relative humidity ranges. The treatment of bulk–surface equilibrium leads to deviations from classical cloud droplet activation behavior as modeled by simplified treatments of the Köhler equation that do not account for bulk–surface partitioning. The treatments for bulk–surface partitioning laid out in this work, when applied to the Köhler equation, are in agreement with measured critical supersaturations of a range of different systems. However, we also find that challenges remain in accurately modeling the growth behavior of certain systems containing small dicarboxylic acids, especially in a predictive manner. Furthermore, it was determined that the thickness of the interfacial phase is a sensitive parameter in this treatment; however, constraining it to a meaningful range allows for predictive modeling of aerosol particle activation into cloud droplets, including cases with consideration of co-condensation of semivolatile organics.</p

Second moment of the pion's distribution amplitude

We present preliminary results from the QCDSF/UKQCD collaborations for the second moment of the pion's distribution amplitude with two flavours of dynamical fermions. We use nonperturbatively determined renormalisation coefficients to convert our results to the MSbar scheme at 5 GeV^2. Employing a linear chiral extrapolation from our large pion masses >550 MeV, we find =0.281(28), leading to a value of a_2=0.236(82) for the second Gegenbauer moment.Comment: 6 pages, 5 figures, 1 table. To appear in: Procs. of the Workshop on Light-Cone QCD and Nonperturbative Hadron Physics 2005 (LC 2005), Cairns, Australia, 200

Spectral quark model and low-energy hadron phenomenology

We propose a spectral quark model which can be applied to low energy hadronic physics. The approach is based on a generalization of the Lehmann representation of the quark propagator. We work at the one-quark-loop level. Electromagnetic and chiral invariance are ensured with help of the gauge technique which provides particular solutions to the Ward-Takahashi identities. General conditions on the quark spectral function follow from natural physical requirements. In particular, the function is normalized, its all positive moments must vanish, while the physical observables depend on negative moments and the so-called log-moments. As a consequence, the model is made finite, dispersion relations hold, chiral anomalies are preserved, and the twist expansion is free from logarithmic scaling violations, as requested of a low-energy model. We study a variety of processes and show that the framework is very simple and practical. Finally, incorporating the idea of vector-meson dominance, we present an explicit construction of the quark spectral function which satisfies all the requirements. The corresponding momentum representation of the resulting quark propagator exhibits only cuts on the physical axis, with no poles present anywhere in the complex momentum space. The momentum-dependent quark mass compares very well to recent lattice calculations. A large number of predictions and relations can be deduced from our approach for such quantities as the pion light-cone wave function, non-local quark condensate, pion transition form factor, pion valence parton distribution function, etc.Comment: revtex, 24 pages, 3 figure

Pion light cone wave function in the non-local NJL model

We use the simple instanton motivated NJL-type model to calculate the leading twist pion light cone wave function. The model consists in employing the momentum dependent quark mass in the quark loop entering the definition of the wave function. The result is analytical up to a solution of a certain algebraic equation. Various properties including the kT dependence of the pion wave function are discussed. The resulting kT integrated wave function is not asymptotic and is in agreement with recent analysis of the CLEO data.Comment: 9 pages, 12 figures, formulas (23-25) corrected, typos correcte

Pion light-cone wave function and pion distribution amplitude in the Nambu-Jona-Lasinio model

We compute the pion light-cone wave function and the pion quark distribution amplitude in the Nambu-Jona-Lasinio model. We use the Pauli-Villars regularization method and as a result the distribution amplitude satisfies proper normalization and crossing properties. In the chiral limit we obtain the simple results, namely phi_pi(x)=1 for the pion distribution amplitude, and = -M / f_pi^2 for the second moment of the pion light-cone wave function, where M is the constituent quark mass and f_pi is the pion decay constant. After the QCD Gegenbauer evolution of the pion distribution amplitude good end-point behavior is recovered, and a satisfactory agreement with the analysis of the experimental data from CLEO is achieved. This allows us to determine the momentum scale corresponding to our model calculation, which is close to the value Q_0 = 313 MeV obtained earlier from the analogous analysis of the pion parton distribution function. The value of is, after the QCD evolution, around (400 MeV)^2. In addition, the model predicts a linear integral relation between the pion distribution amplitude and the parton distribution function of the pion, which holds at the leading-order QCD evolution.Comment: mistake in Eq.(38) correcte

Α-Pinene-Derived organic coatings on acidic sulfate aerosol impacts secondary organic aerosol formation from isoprene in a box model

Fine particulate matter (PM2.5) is known to have an adverse impact on public health and is an important climate forcer. Secondary organic aerosol (SOA) contributes up to 80% of PM2.5 worldwide and multiphase reactions are an important pathway to form SOA. Aerosol-phase state is thought to influence the reactive uptake of gas-phase precursors to aerosol particles by altering diffusion rates within particles. Current air quality models do not include the impact of diffusion-limiting organic coatings on SOA formation. This work examines how α-pinene-derived organic coatings change the predicted formation of SOA from the acid-catalyzed multiphase reactions of isoprene epoxydiols (IEPOX). A box model, with inputs provided from field measurements taken at the Look Rock (LRK) site in Great Smokey Mountains National Park during the 2013 Southern Oxidant and Aerosol Study (SOAS), was modified to incorporate the latest laboratory-based kinetic data accounting for organic coating influences. Including an organic coating influence reduced the modeled reactive uptake when relative humidity was in the 55–80% range, with predicted IEPOX-derived SOA being reduced by up to 33%. Only sensitivity cases with a large increase in Henry's Law values of an order of magnitude or more or in particle reaction rates resulted in the large statistically significant differences form base model performance. These results suggest an organic coating layer could have an impact on IEPOX-derived SOA formation and warrant consideration in regional and global scale models