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Isotope Effects in N2O Photolysis from First Principles : Volume 11, Issue 5 (26/05/2011)

By Schmidt, J. A.

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Book Id: WPLBN0003977108
Format Type: PDF Article :
File Size: Pages 31
Reproduction Date: 2015

Title: Isotope Effects in N2O Photolysis from First Principles : Volume 11, Issue 5 (26/05/2011)  
Author: Schmidt, J. A.
Volume: Vol. 11, Issue 5
Language: English
Subject: Science, Atmospheric, Chemistry
Collections: Periodicals: Journal and Magazine Collection, Copernicus GmbH
Historic
Publication Date:
2011
Publisher: Copernicus Gmbh, Göttingen, Germany
Member Page: Copernicus Publications

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Schinke, R., Johnson, M. S., & Schmidt, J. A. (2011). Isotope Effects in N2O Photolysis from First Principles : Volume 11, Issue 5 (26/05/2011). Retrieved from http://new.worldlibrary.net/


Description
Description: Department of Chemistry, University of Copenhagen, Universitetsparken 5, 2100 Copenhagen Ø, Denmark. For the first time, accurate potential energy surfaces allow N2O cross sections and isotopic fractionation spectra to be derived that are in agreement with available experimental data (without ad hoc shifting), extending knowledge to a much broader range of conditions. Absorption spectra of rare N- and O-isotopologues (15N14N16O, 14N15N16O, 15N216O, 14N217O and 14N218O) calculated using wavepacket propagation are compared to the most abundant isotopologue (14N216O). The fractionation constants as a function of wavelength and temperature are in excellent agreement with experimental data. The study shows that excitations from the 3rd excited bending state, (0,3,0), and the first combination band, (1,1,0), are important for explaining the isotope effect at wavelengths longer than 210 nm. Only a small amount of the mass independent oxygen isotope anomaly observed in atmospheric N2O samples can be explained as arising from photolysis.

Summary
Isotope effects in N2O photolysis from first principles

Excerpt
Assonov, S. S. and Brenninkmeijer, C. A. M.: Reporting small Δ17O values: existing definitions and concepts, Rapid Commun. Mass Spectrom., 19, 627–636, doi:10.1002/rcm.1833, 2005.; Chen, W.-C., Prakash, M. K., and Marcus, R. A.: Isotopomer fractionation in the UV photolysis of N2O: 2. Further comparison of theory and experiment, J. Geophys. Res., 113, D05309, doi:10.1029/2007JD009180, 2008.; Chen, W.-C., Nanbu, S., and Marcus, R. A.: Isotopomer Fractionation in the UV Photolysis of N2O: 3. 3D Ab Initio Surfaces and Anharmonic Effects, J. Phys. Chem. A, 114, 9700–9708, doi:10.1021/jp101691r, 2010.; Cliff, S. S. and Thiemens, M. H.: The 18O/16O and 17O/16O Ratios in Atmospheric Nitrous Oxide: A Mass-Independent Anomaly, Science, 278, 1774–1776, doi:10.1126/science.278.5344.1774, 1997.; Daud, M. N., Balint-Kurti, G. G., and Brown, A.: Ab initio potential energy surfaces, total absorption cross sections, and product quantum state distributions for the low-lying electronic states of N2O, J. Chem. Phys., 122, 054305, doi:10.1063/1.1830436, 2005.; Dunning Jr., T. H.: Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen, J. Chem. Phys., 90, 1007–1023, doi:10.1063/1.456153, 1989.; Forster, P., Ramaswamy, V., Artaxo, P., Berntsen, T., Betts, R., Fahey, D. W., Haywood, J., Lean, J., Lowe, D. C., Myhre, G., Nganga, J., Prinn, R., Raga, G., Schulz, M., and Van Dorland, R.: Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, Cambridge University Press, 2007.; Hopper, D. G.: Ab initio multiple root optimization MCSCF study of the $C_{\infty v}$/$C_s$ excitation spectra and potential energy surfaces of N2O, J. Chem. Phys., 80, 4290–4316, doi:10.1063/1.447260, 1984.; Johnson, M. S., Billing, G. D., Gruodis, A., and Janssen, M. H. M.: Photolysis of Nitrous Oxide Isotopomers Studied by Time-Dependent Hermite Propagation, J. Phys. Chem. A, 105, 8672–8680, doi:10.1021/jp011449x, 2001.; Johnston, J. C., Cliff, S. S., and Thiemens, M. H.: Measurement of multioxygen isotopic (δ18O and $\delta^{17}$O) fractionation factors in the stratospheric sink reactions of nitrous oxide, J. Geophys. Res., 100, 16801–16804, doi:10.1029/95JD01646, 1995.; Kaiser, J. and Röckmann, T.: Absence of isotope exchange in the reaction of N2O + O($^1D$) and the global Δ17O budget of nitrous oxide, Geophys. Res. Lett., 32, L15808, doi:10.1029/2005GL023199, 2005.; Kaiser, J., Röckmann, T., and Brenninkmeijer, C. A. M.: Temperature dependence of isotope fractionation in N2O photolysis, Phys. Chem. Chem. Phys., 4, 4420–4430, doi:10.1039/B204837J, 2002.; Kaiser, J., Röckmann, T., Brenninkmeijer, C. A. M., and Crutzen, P. J.: Wavelength dependence

 

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