The Role of Sulfuric Acid in Atmospheric Nucleation

被引：611

作者：

Sipila, Mikko ^{[1
,2
,3
]}

Berndt, Torsten ^{[1
]}

Petaja, Tuukka ^{[2
]}

Brus, David ^{[4
,5
]}

Vanhanen, Joonas ^{[2
]}

Stratmann, Frank ^{[1
]}

Patokoski, Johanna ^{[2
]}

Mauldin, Roy L., III ^{[6
]}

Hyvarinen, Antti-Pekka ^{[5
]}

Lihavainen, Heikki ^{[5
]}

Kulmala, Markku ^{[2
,7
]}

机构：

[1] Leibniz Inst Tropospharenforsch eV, D-04318 Leipzig, Germany

[2] Univ Helsinki, Dept Phys, FIN-00014 Helsinki, Finland

[3] Univ Helsinki, Helsinki Inst Phys, FIN-00014 Helsinki, Finland

[4] Acad Sci Czech Republic, Inst Chem Proc Fundamentals, Lab Aerosol Chem & Phys, Prague 18502, Czech Republic

[5] Finnish Meteorol Inst, FIN-00101 Helsinki, Finland

[6] Natl Ctr Atmospher Res, Boulder, CO 80307 USA

[7] Stockholm Univ, Dept Appl Environm Sci, S-10691 Stockholm, Sweden

来源：

SCIENCE | 2010年 / 327卷 / 5970期

基金：

芬兰科学院; 欧洲研究理事会;

关键词：

PARTICLE FORMATION; AEROSOL FORMATION; H2SO4; GROWTH; SIZE; NM; MECHANISMS; VAPORS; RATES; SO2;

D O I：

10.1126/science.1180315

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Nucleation is a fundamental step in atmospheric new-particle formation. However, laboratory experiments on nucleation have systematically failed to demonstrate sulfuric acid particle formation rates as high as those necessary to account for ambient atmospheric concentrations, and the role of sulfuric acid in atmospheric nucleation has remained a mystery. Here, we report measurements of new particles ( with diameters of approximately 1.5 nanometers) observed immediately after their formation at atmospherically relevant sulfuric acid concentrations. Furthermore, we show that correlations between measured nucleation rates and sulfuric acid concentrations suggest that freshly formed particles contain one to two sulfuric acid molecules, a number consistent with assumptions that are based on atmospheric observations. Incorporation of these findings into global models should improve the understanding of the impact of secondary particle formation on climate.

引用

页码：1243 / 1246

页数：4

共 31 条

[1] Laboratory studies of particle nucleation:: Initial results for H2SO4, H2O, and NH3 vapors [J].

Ball, SM ;

Hanson, DR ;

Eisele, FL ;

McMurry, PH .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1999, 104 (D19) :23709-23718

[2] Laboratory-measured nucleation rates of sulfuric acid and water binary homogeneous nucleation from the SO2+OHreaction [J].

Benson, David R. ;

Young, Li-Hao ;

Kameel, F. Rifkha ;

Lee, Shan-Hu .

GEOPHYSICAL RESEARCH LETTERS, 2008, 35 (11)

[3] SO2 oxidation products other than H2SO4 as a trigger of new particle formation. Part 1: Laboratory investigations [J].

Berndt, T. ;

Stratmann, F. ;

Braesel, S. ;

Heintzenberg, J. ;

Laaksonen, A. ;

Kulmala, M. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2008, 8 (21) :6365-6374

[4] Rapid formation of sulfuric acid particles at near-atmospheric conditions [J].

Berndt, T ;

Böge, O ;

Stratmann, F ;

Heintzenberg, J ;

Kulmala, M .

SCIENCE, 2005, 307 (5710) :698-700

[5] Formation of atmospheric H2SO4/H2O particles in the absence of organics:: A laboratory study [J].

Berndt, Torsten ;

Boege, Olaf ;

Stratmann, Frank .

GEOPHYSICAL RESEARCH LETTERS, 2006, 33 (15)

[6] Evolution of newly formed aerosol particles in the continental boundary layer:: A case study including OH and H2SO4 measurements [J].

Birmili, W ;

Wiedensohler, A ;

Plass-Dülmer, C ;

Berresheim, H .

GEOPHYSICAL RESEARCH LETTERS, 2000, 27 (15) :2205-2208

[7] MEASUREMENT OF THE GAS-PHASE CONCENTRATION OF H2SO4 AND METHANE SULFONIC-ACID AND ESTIMATES OF H2SO4 PRODUCTION AND LOSS IN THE ATMOSPHERE [J].

EISELE, FL ;

TANNER, DJ .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1993, 98 (D5) :9001-9010

[8] NUCLEATION BY FREE-RADICALS FROM THE PHOTO-OXIDATION OF SULFUR-DIOXIDE IN AIR [J].

FRIEND, JP ;

BARNES, RA ;

VASTA, RM .

JOURNAL OF PHYSICAL CHEMISTRY, 1980, 84 (19) :2423-2436

[9] Estimating nanoparticle growth rates from size-dependent charged fractions: Analysis of new particle formation events in Mexico City [J].

Iida, Kenjiro ;

Stolzenburg, Mark R. ;

McMurry, Peter H. ;

Smith, James N. .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2008, 113 (D5)

[10] ON THE RELATION BETWEEN NUCLEATION WORK, NUCLEUS SIZE, AND NUCLEATION RATE [J].

KASHCHIEV, D .

JOURNAL OF CHEMICAL PHYSICS, 1982, 76 (10) :5098-5102

← 1 2 3 4 →