Modeling Rayleigh Scattering of Aerosol Particles

被引:11
作者
Harczuk, Ignat [1 ]
Vahtras, Olav [1 ]
Agren, Hans [1 ]
机构
[1] KTH Royal Inst Technol, Div Theoret Chem & Biol, Sch Biotechnol, SE-10691 Stockholm, Sweden
关键词
ATMOSPHERIC IMPLICATION; SULFURIC-ACID; MOLECULAR-DYNAMICS; OXALIC-ACID; CLUSTERS; NUCLEATION; HYDRATION; FIELDS; MOTION;
D O I
10.1021/acs.jpcb.6b02278
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Rayleigh scattering of naturally polarized light was studied for systems with atmospheric relevance representing growing water clusters with adsorbed cis-pinonic acid. The scattering intensity was computed from the static and dynamical polarizabilities of the clusters obtained by a recently derived methodology for classical polarizabilities, in which Applequist equations for interacting polarizable dipoles are used together with point-dipoles and polarizabilities obtained by quantum chemistry and decomposed into the atomic domain by the so-called LoProp transformation generalized for frequency dependence. The Applequist interaction was found to yield scattering intensities 20% larger for a cluster consisting of 1000 water molecules, as compared to the method where all of the polarizabilities of molecules are added without interactions. It was confirmed that scattering intensity depends quadratically on the number of water molecules in the cluster, and that it also increases quadratically with increase in the mass constituent of the foreign substance. The adsorption of the cis-pinonic acid increases the contribution to the scattering intensity stemming from the anisotropic polarizability, as compared to the isotropic contribution. The ramifications of the method in predicting Rayleigh scattering and the earth's albedo with respect to man-made and natural gas emission are briefly discussed.
引用
收藏
页码:4296 / 4301
页数:6
相关论文
共 25 条
[1]   The Dalton quantum chemistry program system [J].
Aidas, Kestutis ;
Angeli, Celestino ;
Bak, Keld L. ;
Bakken, Vebjorn ;
Bast, Radovan ;
Boman, Linus ;
Christiansen, Ove ;
Cimiraglia, Renzo ;
Coriani, Sonia ;
Dahle, Pal ;
Dalskov, Erik K. ;
Ekstrom, Ulf ;
Enevoldsen, Thomas ;
Eriksen, Janus J. ;
Ettenhuber, Patrick ;
Fernandez, Berta ;
Ferrighi, Lara ;
Fliegl, Heike ;
Frediani, Luca ;
Hald, Kasper ;
Halkier, Asger ;
Hattig, Christof ;
Heiberg, Hanne ;
Helgaker, Trygve ;
Hennum, Alf Christian ;
Hettema, Hinne ;
Hjertenaes, Eirik ;
Host, Stinne ;
Hoyvik, Ida-Marie ;
Iozzi, Maria Francesca ;
Jansik, Branislav ;
Jensen, Hans Jorgen Aa. ;
Jonsson, Dan ;
Jorgensen, Poul ;
Kauczor, Joanna ;
Kirpekar, Sheela ;
Kjrgaard, Thomas ;
Klopper, Wim ;
Knecht, Stefan ;
Kobayashi, Rika ;
Koch, Henrik ;
Kongsted, Jacob ;
Krapp, Andreas ;
Kristensen, Kasper ;
Ligabue, Andrea ;
Lutnaes, Ola B. ;
Melo, Juan I. ;
Mikkelsen, Kurt V. ;
Myhre, Rolf H. ;
Neiss, Christian .
WILEY INTERDISCIPLINARY REVIEWS-COMPUTATIONAL MOLECULAR SCIENCE, 2014, 4 (03) :269-284
[2]   ATOM DIPOLE INTERACTION MODEL FOR MOLECULAR POLARIZABILITY - APPLICATION TO POLYATOMIC-MOLECULES AND DETERMINATION OF ATOM POLARIZABILITIES [J].
APPLEQUIST, J ;
CARL, JR ;
FUNG, KK .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1972, 94 (09) :2952-+
[3]   MOLECULAR VIBRATIONAL AND ROTATIONAL MOTION IN STATIC AND DYNAMIC ELECTRIC-FIELDS [J].
BISHOP, DM .
REVIEWS OF MODERN PHYSICS, 1990, 62 (02) :343-374
[4]   On the properties and atmospheric implication of amine-hydrated clusters [J].
Chen, Jiao ;
Jiang, Shuai ;
Miao, Shou-Kui ;
Peng, Xiu-Qiu ;
Ma, Yan ;
Wang, Chun-Yu ;
Zhang, Miao-Miao ;
Liu, Yi-Rong ;
Huang, Wei .
RSC ADVANCES, 2015, 5 (111) :91500-91515
[5]   Drought under global warming: a review [J].
Dai, Aiguo .
WILEY INTERDISCIPLINARY REVIEWS-CLIMATE CHANGE, 2011, 2 (01) :45-65
[6]   Rayleigh light scattering properties of atmospheric molecular clusters consisting of sulfuric acid and bases [J].
Elm, Jonas ;
Norman, Patrick ;
Mikkelsen, Kurt V. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2015, 17 (24) :15701-15709
[7]   Computational study of the Rayleigh light scattering properties of atmospheric pre-nucleation clusters [J].
Elm, Jonas ;
Norman, Patrick ;
Bilde, Merete ;
Mikkelsen, Kurt V. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2014, 16 (22) :10883-10890
[8]   Local properties of quantum chemical systems:: The LoProp approach [J].
Gagliardi, L ;
Lindh, R ;
Karlström, G .
JOURNAL OF CHEMICAL PHYSICS, 2004, 121 (10) :4494-4500
[9]   Hyperpolarizabilities of extended molecular mechanical systems [J].
Harczuk, Ignat ;
Vahtras, Olav ;
Agren, Hans .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2016, 18 (12) :8710-8722
[10]   Frequency-dependent force fields for QMMM calculations [J].
Harczuk, Ignat ;
Vahtras, Olav ;
Agren, Hans .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2015, 17 (12) :7800-7812