A simple model to estimate atmospheric concentrations of aerosol chemical species based on snow core chemistry at Summit, Greenland

A simple model is presented to estimate atmospheric concentrations of chemical species that exist primarily as aerosols based on snow core/ice core chemistry at Summit, Greenland. The model considers the processes of snow, fog, and dry deposition. The deposition parameters for each of the processes are estimated for SO42− and Ca2+ and are based on experiments conducted during the 1993 and 1994 summer field seasons. The seasonal mean atmospheric concentrations are estimated based on the deposition parameters and snow cores obtained during the field seasons. The ratios of the estimated seasonal mean airborne concentration divided by the measured mean concentration ( ) for SO42− over the 1993 and 1994 field seasons are 0.85 and 0.95, respectively. The ratios for Ca2+ are 0.45 and 0.90 for the 1993 and 1994 field seasons. The uncertainties in the estimated atmospheric concentrations range from 30% to 40% and are due to variability in the input parameters. The model estimates the seasonal mean atmospheric SO42− and Ca2+ concentrations to within 15% and 55%, respectively. Although the model is not directly applied to ice cores, the application of the model to ice core chemical signals is briefly discussed

Modeling of the processing and removal of trace gas and aerosol species by Arctic radiation fogs and comparison with measurements

A Lagrangian radiation fog model is applied to a fog event at Summit, Greenland. The model simulates the formation and dissipation of fog. Included in the model are detailed gas and aqueous phase chemistry, and deposition of chemical species with fog droplets. Model predictions of the gas phase concentrations of H2O2, HCOOH, SO2, and HNO3 as well as the fog fluxes of S(VI), N(V), H2O2, and water are compared with measurements. The predicted fluxes of S(VI), N(V), H2O2, and fog water generally agree with measured values. Model results show that heterogeneous SO2 oxidation contributes to approximately 40% of the flux of S(VI) for the modeled fog event, with the other 60% coming from preexisting sulfate aerosol. The deposition of N(V) with fog includes contributions from HNO3 and NO2 initially present in the air mass. HNO3 directly partitions into the aqueous phase to create N(V), and NO2 forms N(V) through reaction with OH and the nighttime chemistry set of reactions which involves N2O5 and water vapor. PAN contributes to N(V) by gas phase decomposition to NO2, and also by direct aqueous phase decomposition. The quantitative contributions from each path are uncertain since direct measurements of PAN and NO2 are not available for the fog event. The relative contributions are discussed based on realistic ranges of atmospheric concentrations. Model results suggest that in addition to the aqueous phase partitioning of the initial HNO3 present in the air mass, the gas phase decomposition of PAN and subsequent reactions of NO2 with OH as well as nighttime nitrate chemistry may play significant roles in depositing N(V) with fog. If a quasi-liquid layer exists on snow crystals, it is possible that the reactions taking place in fog droplets also occur to some extent in clouds as well as at the snow surface

Quantum critical dynamics of a S = 1/2 antiferromagnetic Heisenberg chain studied by 13C-NMR spectroscopy

We present a 13C-NMR study of the magnetic field driven transition to complete polarization of the S=1/2 antiferromagnetic Heisenberg chain system copper pyrazine dinitrate Cu(C_4H_4N_2)(NO_3)_2 (CuPzN). The static local magnetization as well as the low-frequency spin dynamics, probed via the nuclear spin-lattice relaxation rate 1/T_1, were explored from the low to the high field limit and at temperatures from the quantum regime (k_B T << J) up to the classical regime (k_B T >> J). The experimental data show very good agreement with quantum Monte Carlo calculations over the complete range of parameters investigated. Close to the critical field, as derived from static experiments, a pronounced maximum in 1/T_1 is found which we interpret as the finite-temperature manifestation of a diverging density of zero-energy magnetic excitations at the field-driven quantum critical point.Comment: 5 pages, 4 figure