Computational study of the Rayleigh light scattering properties of atmospheric pre-nucleation clusters

Jonas Elm; Patrick Norman; Merete Bilde; Kurt Valentin Mikkelsen

doi:10.1039/c4cp01206b

Computational study of the Rayleigh light scattering properties of atmospheric pre-nucleation clusters

Jonas Elm^*, Patrick Norman, Merete Bilde, Kurt Valentin Mikkelsen

^*Corresponding author af dette arbejde

Kemisk Institut

22 Citationer (Scopus)

Abstract

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

Originalsprog	Engelsk
Tidsskrift	Physical Chemistry Chemical Physics
Vol/bind	16
Udgave nummer	22
Sider (fra-til)	10883-10890
Antal sider	8
ISSN	1463-9076
DOI	https://doi.org/10.1039/c4cp01206b
Status	Udgivet - 2014

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10.1039/c4cp01206b

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title = "Computational study of the Rayleigh light scattering properties of atmospheric pre-nucleation clusters",

abstract = "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",

author = "Jonas Elm and Patrick Norman and Merete Bilde and Mikkelsen, {Kurt Valentin}",

year = "2014",

doi = "10.1039/c4cp01206b",

language = "English",

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pages = "10883--10890",

journal = "Physical Chemistry Chemical Physics",

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TY - JOUR

T1 - Computational study of the Rayleigh light scattering properties of atmospheric pre-nucleation clusters

AU - Elm, Jonas

AU - Norman, Patrick

AU - Bilde, Merete

AU - Mikkelsen, Kurt Valentin

PY - 2014

Y1 - 2014

N2 - 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

AB - 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

U2 - 10.1039/c4cp01206b

DO - 10.1039/c4cp01206b

M3 - Journal article

C2 - 24763512

AN - SCOPUS:84900825721

SN - 1463-9076

VL - 16

SP - 10883

EP - 10890

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

IS - 22

ER -

Computational study of the Rayleigh light scattering properties of atmospheric pre-nucleation clusters

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