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1 Administration, Department of Chemistry, Faculty of Science, Københavns Universitet 2 Department of Chemistry, Faculty of Science, Københavns Universitet 3 Linköping University 4 Institut for Kemi, Aarhus Universitet 5 Department of Chemistry, Faculty of Science, Københavns Universitet 6 Administration, Department of Chemistry, Faculty of Science, Københavns Universitet
The Rayleigh and hyper Rayleigh scattering properties of the binary (H 2SO4)(H2O)n and ternary (H 2SO4)(NH3)(H2O)n clusters are investigated using a quantum mechanical response theory approach. The molecular Rayleigh scattering intensities are expressed using the dipole polarizability α and hyperpolarizability β tensors. Using density functional theory, we elucidate the effect of cluster morphology on the scattering properties using a combinatorial sampling approach. We find that the Rayleigh scattering intensity depends quadratically on the number of water molecules in the cluster and that a single ammonia molecule is able to induce a high anisotropy, which further increases the scattering intensity. The hyper Rayleigh scattering activities are found to be extremely low. This study presents the first attempt to map the scattering of atmospheric molecular clusters using a bottom-up approach. This journal is © the Partner Organisations 2014.
Physical Chemistry Chemical Physics, 2014, Vol 16, Issue 22, p. 10883-10890
DENSITY-FUNCTIONAL THEORY; GAS-PHASE HYDRATION; SULFURIC-ACID; PARTICLE FORMATION; AB-INITIO; AEROSOL NUCLEATION; MOLECULAR CLUSTERS; EARTHS ATMOSPHERE; ORGANIC-ACIDS; WATER CLUSTERS
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