Experimental Observation of Strongly Bound Dimers of Sulfuric Acid: Application to Nucleation in the Atmosphere

Tuukka Petaja; Mikko Sipila; Pauli Paasonen; Tuomo Nieminen; Theo Kurten; Ismael K. Ortega; Frank Stratmann; Hanna Vehkamaki; Torsten Berndt; Markku Kulmala

doi:10.1103/physrevlett.106.228302

Experimental Observation of Strongly Bound Dimers of Sulfuric Acid: Application to Nucleation in the Atmosphere

Tuukka Petaja, Mikko Sipila, Pauli Paasonen, Tuomo Nieminen, Theo Kurten, Ismael K. Ortega, Frank Stratmann, Hanna Vehkamaki, Torsten Berndt, Markku Kulmala

Department of Chemistry

55 Citations (Scopus)

Abstract

Sulfuric acid is a key compound in atmospheric nucleation. Here we report on the observation of a close-to-collision-limited sulfuric acid dimer formation in atmospherically relevant laboratory conditions in the absence of measurable quantities of ammonia or organics. The observed dimer formation rate was clearly higher than the measured new particle formation rate at ∼1.5nm suggesting that the rate limiting step for the nucleation takes place after the dimerization step. The quantum chemical calculations suggested that even in the ultraclean conditions there exist (a) stabilizing compound(s) with (a) concentration(s) high enough to prevent the dimer evaporation. Such a stabilizing compound should be abundant enough in any natural environment and would therefore not limit the formation of sulfuric acid dimers in the atmosphere.

Original language	English
Journal	Physical Review Letters
Volume	106
Issue number	22
ISSN	0031-9007
DOIs	https://doi.org/10.1103/physrevlett.106.228302
Publication status	Published - 1 Jun 2011

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title = "Experimental Observation of Strongly Bound Dimers of Sulfuric Acid: Application to Nucleation in the Atmosphere",

abstract = "Sulfuric acid is a key compound in atmospheric nucleation. Here we report on the observation of a close-to-collision-limited sulfuric acid dimer formation in atmospherically relevant laboratory conditions in the absence of measurable quantities of ammonia or organics. The observed dimer formation rate was clearly higher than the measured new particle formation rate at ∼1.5nm suggesting that the rate limiting step for the nucleation takes place after the dimerization step. The quantum chemical calculations suggested that even in the ultraclean conditions there exist (a) stabilizing compound(s) with (a) concentration(s) high enough to prevent the dimer evaporation. Such a stabilizing compound should be abundant enough in any natural environment and would therefore not limit the formation of sulfuric acid dimers in the atmosphere.",

author = "Tuukka Petaja and Mikko Sipila and Pauli Paasonen and Tuomo Nieminen and Theo Kurten and Ortega, {Ismael K.} and Frank Stratmann and Hanna Vehkamaki and Torsten Berndt and Markku Kulmala",

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doi = "10.1103/physrevlett.106.228302",

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T1 - Experimental Observation of Strongly Bound Dimers of Sulfuric Acid: Application to Nucleation in the Atmosphere

AU - Petaja, Tuukka

AU - Sipila, Mikko

AU - Paasonen, Pauli

AU - Nieminen, Tuomo

AU - Kurten, Theo

AU - Ortega, Ismael K.

AU - Stratmann, Frank

AU - Vehkamaki, Hanna

AU - Berndt, Torsten

AU - Kulmala, Markku

PY - 2011/6/1

Y1 - 2011/6/1

N2 - Sulfuric acid is a key compound in atmospheric nucleation. Here we report on the observation of a close-to-collision-limited sulfuric acid dimer formation in atmospherically relevant laboratory conditions in the absence of measurable quantities of ammonia or organics. The observed dimer formation rate was clearly higher than the measured new particle formation rate at ∼1.5nm suggesting that the rate limiting step for the nucleation takes place after the dimerization step. The quantum chemical calculations suggested that even in the ultraclean conditions there exist (a) stabilizing compound(s) with (a) concentration(s) high enough to prevent the dimer evaporation. Such a stabilizing compound should be abundant enough in any natural environment and would therefore not limit the formation of sulfuric acid dimers in the atmosphere.

AB - Sulfuric acid is a key compound in atmospheric nucleation. Here we report on the observation of a close-to-collision-limited sulfuric acid dimer formation in atmospherically relevant laboratory conditions in the absence of measurable quantities of ammonia or organics. The observed dimer formation rate was clearly higher than the measured new particle formation rate at ∼1.5nm suggesting that the rate limiting step for the nucleation takes place after the dimerization step. The quantum chemical calculations suggested that even in the ultraclean conditions there exist (a) stabilizing compound(s) with (a) concentration(s) high enough to prevent the dimer evaporation. Such a stabilizing compound should be abundant enough in any natural environment and would therefore not limit the formation of sulfuric acid dimers in the atmosphere.

U2 - 10.1103/physrevlett.106.228302

DO - 10.1103/physrevlett.106.228302

M3 - Journal article

C2 - 21702637

SN - 0031-9007

VL - 106

JO - Physical Review Letters

JF - Physical Review Letters

IS - 22

ER -

Experimental Observation of Strongly Bound Dimers of Sulfuric Acid: Application to Nucleation in the Atmosphere

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