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

The contributions of snow, fog, and dry deposition to the summer flux of anions and cations at Summit, Greenland

Experiments were performed during the period May–July of 1993 at Summit, Greenland. Aerosol mass size distributions as well as daily average concentrations of several anionic and cationic species were measured. Dry deposition velocities for SO42− were estimated using surrogate surfaces (symmetric airfoils) as well as impactor data. Real-time concentrations of particles greater than 0.5 μm and greater than 0.01 μm were measured. Snow and fog samples from nearly all of the events occurring during the field season were collected. Filter sampler results indicate that SO42− is the dominant aerosol anion species, with Na+, NH4+, and Ca2+being the dominant cations. Impactor results indicate that MSA and SO42− have similar mass size distributions. Furthermore, MSA and SO42− have mass in both the accumulation and coarse modes. A limited number of samples for NH4+ indicate that it exists in the accumulation mode. Na, K, Mg, and Ca exist primarily in the coarse mode. Dry deposition velocities estimated from impactor samples and a theory for dry deposition to snow range from 0.017 cm/s +/− 0.011 cm/s for NH4+ to 0.110 cm/s +/− 0.021 cm/s for Ca. SO42− dry deposition velocity estimates using airfoils are in the range 0.023 cm/s to 0.062 cm/s, as much as 60% greater than values calculated using the airborne size distribution data. The rough agreement between the airfoil and impactor-estimated dry deposition velocities suggests that the airfoils may be used to approximate the dry deposition to the snow surface. Laser particle counter (LPC) results show that particles \u3e 0.5 μm in diameter efficiently serve as nuclei to form fog droplets. Condensation nuclei (CN) measurements indicate that particles \u3c 0.5 μm are not as greatly affected by fog. Furthermore, impactor measurements suggest that from 50% to 80% of the aerosol SO42−serves as nuclei for fog droplets. Snow deposition is the dominant mechanism transporting chemicals to the ice sheet. For NO3−, a species that apparently exists primarily in the gas phase as HNO3(g), 93% of the seasonal inventory (mass of a deposited chemical species per unit area during the season) is due to snow deposition, which suggests efficient scavenging of HNO3(g) by snowflakes. The contribution of snow deposition to the seasonal inventories of aerosols ranges from 45% for MSA to 76% for NH4+. The contribution of fog to the seasonal inventories ranges from 13% for Na+ and Ca2+ to 26% and 32% for SO42− and MSA. The dry deposition contribution to the seasonal inventories of the aerosol species is as low as 5% for NH4+ and as high as 23% for MSA. The seasonal inventory estimations do not take into consideration the spatial variability caused by blowing and drifting snow. Overall, results indicate that snow deposition of chemical species is the dominant flux mechanism during the summer at Summit and that all three deposition processes should be considered when estimating atmospheric concentrations based on ice core chemical signals

Two inequivalent sublattices and orbital ordering in MnV2O4 studied by 51V NMR

We report detailed 51V NMR spectra in a single crystal of MnV2O4. The vanadium spectrum reveals two peaks in the orbitally ordered state, which arise from different internal hyperfine fields at two different V sublattices. These internal fields evolve smoothly with externally applied field, and show no change in structure that would suggest a change of the orbital ordering. The result is consistent with the orbital ordering model recently proposed by Sarkar et al. [Phys. Rev. Lett. 102, 216405 (2009)] in which the same orbital that is a mixture of t_2g orbitals rotates by about 45$^\circ$ alternately within and between orbital chains in the I4_1/a tetragonal space group.Comment: 4 pages, 4 figures, title changed, published in PRB as a rapid com

Spin susceptibility of charge ordered YBa2Cu3Oy across the upper critical field

The value of the upper critical field Hc2, a fundamental characteristic of the superconducting state, has been subject to strong controversy in high-Tc copper-oxides. Since the issue has been tackled almost exclusively by macroscopic techniques so far, there is a clear need for local-probe measurements. Here, we use 17O NMR to measure the spin susceptibility $\chi_{spin}$ of the CuO2 planes at low temperature in charge ordered YBa2Cu3Oy. We find that $\chi_{spin}$ increases (most likely linearly) with magnetic field H and saturates above field values ranging from 20 to 40 T. This result is consistent with Hc2 values claimed by G. Grissonnanche et al. [Nat. Commun. 5, 3280 (2014)] and with the interpretation that the charge-density-wave (CDW) reduces Hc2 in underdoped YBa2Cu3Oy. Furthermore, the absence of marked deviation in $\chi_{spin}(H)$ at the onset of long-range CDW order indicates that this Hc2 reduction and the Fermi-surface reconstruction are primarily rooted in the short-range CDW order already present in zero field, not in the field-induced long-range CDWorder. Above Hc2, the relatively low values of $\chi_{spin}$ at T=2 K show that the pseudogap is a ground-state property, independent of the superconducting gap.Comment: To appea

Evidence for Skyrmion crystallization from NMR relaxation experiments

A resistively detected NMR technique was used to probe the two-dimensional electron gas in a GaAs/AlGaAs quantum well. The spin-lattice relaxation rate $(1/T_{1})$ was extracted at near complete filling of the first Landau level by electrons. The nuclear spin of $^{75}$As is found to relax much more efficiently with $T\to 0$ and when a well developed quantum Hall state with $R_{xx}\simeq 0$ occurs. The data show a remarkable correlation between the nuclear spin relaxation and localization. This suggests that the magnetic ground state near complete filling of the first Landau level may contain a lattice of topological spin texture, i.e. a Skyrmion crystal