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 for this work

Department of Chemistry

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

39 Citations (Scopus)

Abstract

The Rayleigh and hyper Rayleigh scattering properties of the binary (H2SO4)(H2O)(n) and ternary (H2SO4)(NH3)(H2O) n clusters are investigated using a quantum mechanical response theory approach. The molecular Rayleigh scattering intensities are expressed using the dipole polarizability alpha and hyperpolarizability beta 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.

Original language	English
Journal	Physical Chemistry Chemical Physics
Volume	16
Issue	22
Pages (from-to)	10883-10890
Number of pages	8
ISSN	1463-9076
DOIs	https://doi.org/10.1039/c4cp01206b
Publication status	Published - 2014

Keywords

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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10.1039/c4cp01206b

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@article{45dca2776f194b17908c058c996c8a15,

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 (H2SO4)(H2O)(n) and ternary (H2SO4)(NH3)(H2O) n clusters are investigated using a quantum mechanical response theory approach. The molecular Rayleigh scattering intensities are expressed using the dipole polarizability alpha and hyperpolarizability beta 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.",

keywords = "DENSITY-FUNCTIONAL THEORY, GAS-PHASE HYDRATION, SULFURIC-ACID, PARTICLE FORMATION, AB-INITIO, AEROSOL NUCLEATION, MOLECULAR CLUSTERS, EARTHS ATMOSPHERE, ORGANIC-ACIDS, WATER CLUSTERS",

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

year = "2014",

doi = "10.1039/c4cp01206b",

language = "English",

volume = "16",

pages = "10883--10890",

journal = "Physical Chemistry Chemical Physics",

issn = "1463-9076",

publisher = "Royal Society of Chemistry",

number = "22",

}

Computational study of the Rayleigh light scattering properties of atmospheric pre-nucleation clusters. / Elm, Jonas; Norman, Patrick; Bilde, Merete et al.
In: Physical Chemistry Chemical Physics, Vol. 16, No. 22, 2014, p. 10883-10890.

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

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 (H2SO4)(H2O)(n) and ternary (H2SO4)(NH3)(H2O) n clusters are investigated using a quantum mechanical response theory approach. The molecular Rayleigh scattering intensities are expressed using the dipole polarizability alpha and hyperpolarizability beta 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.

AB - The Rayleigh and hyper Rayleigh scattering properties of the binary (H2SO4)(H2O)(n) and ternary (H2SO4)(NH3)(H2O) n clusters are investigated using a quantum mechanical response theory approach. The molecular Rayleigh scattering intensities are expressed using the dipole polarizability alpha and hyperpolarizability beta 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.

KW - DENSITY-FUNCTIONAL THEORY

KW - GAS-PHASE HYDRATION

KW - SULFURIC-ACID

KW - PARTICLE FORMATION

KW - AB-INITIO

KW - AEROSOL NUCLEATION

KW - MOLECULAR CLUSTERS

KW - EARTHS ATMOSPHERE

KW - ORGANIC-ACIDS

KW - WATER CLUSTERS

U2 - 10.1039/c4cp01206b

DO - 10.1039/c4cp01206b

M3 - Journal article

C2 - 24763512

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

Abstract

Keywords

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