Abstract. The isotopically substituted nitrous oxide species 14N14NO, 15N14NO, 14N15NO and 15N15NO were investigated by ultra-violet (UV) absorption spectroscopy. High precision cross sections were obtained for the wavelength range 181 to 218nm at temperatures of 233 and 283K. These data are used to calculate photolytic isotopic fractionation constants as a function of wavelength. The fractionation constants were used in a three-dimensional chemical transport model in order to simulate the actual fractionation of N2O in the stratosphere, and the results were found to be in good agreement with field studies.
Using cloud data from MODIS we investigate the response of cloud microphysics to sudden decreases in galactic cosmic radiation – Forbush decreases – and find responses in effective emissivity, cloud fraction, liquid water content, and optical thickness above the 2–3 sigma level 6–9 days after the minimum in atmospheric ionization and less significant responses for effective radius and cloud condensation nuclei (<2 sigma). The magnitude of the signals agree with derived values, based on simple equations for atmospheric parameters. Furthermore principal components analysis gives a total significance of the signal of 3.1 sigma. We also see a correlation between total solar irradiance and strong Forbush decreases but a clear mechanism connecting this to cloud properties is lacking. There is no signal in the UV radiation. The responses of the parameters correlate linearly with the reduction in the cosmic ray ionization. These results support the suggestion that ions play a significant role in the life-cycle of clouds
Abstract. In order to elucidate the effect of galactic cosmic rays on cloud formation, we investigate the optical response of marine aerosols to Forbush decreases – abrupt decreases in galactic cosmic rays – by means of modeling. We vary the nucleation rate of new aerosols, in a sectional coagulation and condensation model, according to changes in ionization by the Forbush decrease. From the resulting size distribution we then calculate the aerosol optical thickness and Angstrom exponent, for the wavelength pairs 350, 450 nm and 550, 900 nm. For the shorter wavelength pair we observe a change in Angstrom exponent, following the Forbush Decrease, of −6 to +3% in the cases with atmospherically realistic output parameters. For some parameters we also observe a delay in the change of Angstrom exponent, compared to the maximum of the Forbush decrease, which is caused by different sensitivities of the probing wavelengths to changes in aerosol number concentration and size. For the long wavelengths these changes are generally smaller. The types and magnitude of change is investigated for a suite of nucleation rates, condensable gas production rates, and aerosol loss rates. Furthermore we compare the model output with observations of 5 of the largest Forbush decreases after year 2000. For the 350, 450 nm pair we use AERONET data and find a comparable change in signal while the Angstrom Exponent is lower in the model than in the data, due to AERONET being mainly sampled over land. For 550, 900 nm we compare with both AERONET and MODIS and find little to no response in both model and observations. In summary our study shows that the optical properties of aerosols show a distinct response to Forbush Decreases, assuming that the nucleation of fresh aerosols is driven by ions. Shorter wavelengths seem more favorable for observing these effects and great care should be taken when analyzing observations, in order to avoid the signal being drowned out by noise.
The kinetic isotope effects (KIEs) have been studied in the reactions of chlorine and bromine atoms with four
ethene isotopologues (C2H4, 13C2H4, C2D4, and C2H3D) using FTIR spectroscopy and the relative rate technique.
Halogen atoms were produced by the photolysis of Cl2 and Br2. For chlorine the KIEs, defined as k
C
2
H
4
/k
x
,
were: 0.738 ± 0.024 (C2D4), 0.853 ± 0.037 (C2H3D), and 1.061 ± 0.023 (13C2H4) and for bromine: 0.817
± 0.016 (C2D4), 1.09 ± 0.13 (C2H3D), and 1.1172 ± 0.0053 (13C2H4). Uncertainties are given as 2σ. These
results are interpreted in terms of the fate of the atom−molecule adduct. The implications of the results to
atmospheric chemistry are described.
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