Laboratory studies of particle nucleation: Initial results for H2SO4, H2O, and NH3 vapors

Ball, S. M.; Hanson, David R.; Eisele, F. L.; McMurry, Peter H.

doi:10.1029/1999jd900411

Cited by 346 publications

(526 citation statements)

References 24 publications

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“…[16][17][18] The presence of ammonia (NH 3 ) can stabilize nucleating clusters, and enhance nucleation by orders of magnitude. [19][20][21][22][23][24] However, even taking into account this effect, atmospheric concentrations of H 2 SO 4 and NH 3 are often not sufficient to explain nucleation rates in the atmosphere. 23 Amines have recently been recognized as additional bases that can participate in NPF.…”

Section: Introductionmentioning

confidence: 99%

New particle formation and growth from methanesulfonic acid, trimethylamine and water

Chen

Ezell

Arquero

et al. 2015

Phys. Chem. Chem. Phys.

110

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New particle formation from gas-to-particle conversion represents a dominant source of atmospheric particles and affects radiative forcing, climate and human health. The species involved in new particle formation and the underlying mechanisms remain uncertain. Although sulfuric acid is commonly recognized as driving new particle formation, increasing evidence suggests the involvement of other species. Here we study particle formation and growth from methanesulfonic acid, trimethylamine and water at reaction times from 2.3 to 32 s where particles are 2-10 nm in diameter using a newly designed and tested flow system. The flow system has multiple inlets to facilitate changing the mixing sequence of gaseous precursors. The relative humidity and precursor concentrations, as well as the mixing sequence, are varied to explore their effects on particle formation and growth in order to provide insight into the important mechanistic steps. We show that water is involved in the formation of initial clusters, greatly enhancing their formation as well as growth into detectable size ranges. A kinetics box model is developed that quantitatively reproduces the experimental data under various conditions. Although the proposed scheme is not definitive, it suggests that incorporating such mechanisms into atmospheric models may be feasible in the near future.

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Section: Introductionmentioning

confidence: 99%

New particle formation and growth from methanesulfonic acid, trimethylamine and water

Chen

Ezell

Arquero

et al. 2015

Phys. Chem. Chem. Phys.

110

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show abstract

“…ChemCorrespondence to: S.-H. Lee (slee19@kent.edu) ical analysis of aerosol composition also showed that newly formed atmospheric aerosol particles indeed contain ammonium (NH + 4 ) and sulfate (SO 2− 4 ) along with other components . Laboratory nucleation observations (Ball et al, 1999;Benson et al, 2009) further demonstrated that NH 3 can enhance sulfuric acid and water homogeneous nucleation (Merikanto et al, 2007).…”

Section: Introductionmentioning

confidence: 98%

A Chemical Ionization Mass Spectrometer for ambient measurements of Ammonia

et al. 2010

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Abstract. This study presents a chemical ionization mass spectrometer (CIMS) for fast response, in-situ measurements of gas phase ammonia (NH 3 ). The NH 3 background level detected with the CIMS ranged between 0.3-1 ppbv, with an uncertainty of 30 pptv under optimized conditions. The instrument sensitivity varied from 4-25 Hz/pptv for >1 MHz of reagent ion signals (protonated ethanol ions), with a 30% uncertainty estimated based on variability in calibration signals. The CIMS detection limit for NH 3 was ∼60 pptv at a 1 min integration time (3 sigma). The CIMS time response was <30 s. This new NH 3 -CIMS has been used for ambient measurements in Kent, Ohio, for several weeks throughout three seasons. The measured NH 3 mixing ratios were usually at the sub-ppbv level and higher in spring (200 ± 120 pptv) than in winter (60 ± 75 pptv) and fall (150 ± 80 pptv). High emissions of SO 2 from power plants in this region, and thus possible high acidity of aerosol particles, may explain these low NH 3 mixing ratios in general.

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“…Ammoniated aerosols are a dominant component of inorganic aerosol mass in both clean and urban regions (Jimenez et al, 2009). Gas-phase NH 3 measurements are crucial for understanding aerosol nucleation and new particle formation (Ball et al, 1999;Hanson and Eisele, 2002;McMurry et al, 2005;Benson et al, 2011), which facilitate long-range transport of aerosol ammonium and nitrate (Nowak et al, 2007;Pinder et al, 2008). Ammoniated sulfate aerosols also play an important role in cirrus cloud nucleation (Tabazadeh and Toon, 1998;Wang et al, 2008), and aerosol-cloud interactions have significant yet highly uncertain radiative effects on climate (Adams et al, 2001;Martin et al, 2004;Solomon et al, 2007).…”

Section: Introductionmentioning

confidence: 99%

Open-path, quantum cascade-laser-based sensor for high-resolution atmospheric ammonia measurements

et al. 2014

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Abstract. We demonstrate a compact, open-path, quantum cascade-laser-based atmospheric ammonia sensor operating at 9.06 µm for high-sensitivity, high temporal resolution, ground-based measurements. Atmospheric ammonia (NH 3 ) is a gas-phase precursor to fine particulate matter, with implications for air quality and climate change. Currently, NH 3 sensing challenges have led to a lack of widespread in situ measurements. Our open-path sensor configuration minimizes sampling artifacts associated with NH 3 surface adsorption onto inlet tubing and reduced pressure sampling cells, as well as condensed-phase partitioning ambiguities. Multi-harmonic wavelength modulation spectroscopy allows for selective and sensitive detection of atmospheric pressurebroadened absorption features. An in-line ethylene reference cell provides real-time calibration (±20 % accuracy) and normalization for instrument drift under rapidly changing field conditions. The sensor has a sensitivity and noise-equivalent limit (1σ ) of 0.15 ppbv NH 3 at 10 Hz, a mass of ∼ 5 kg and consumes ∼ 50 W of electrical power. The total uncertainty in NH 3 measurements is 0.20 ppbv NH 3 ± 10 %, based on a spectroscopic calibration method. Field performance of this open-path NH 3 sensor is demonstrated, with 10 Hz time resolution and a large dynamic response for in situ NH 3 measurements. This sensor provides the capabilities for improved in situ gas-phase NH 3 sensing relevant for emission source characterization and flux measurements.

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Laboratory studies of particle nucleation: Initial results for H₂SO₄, H₂O, and NH₃ vapors

Cited by 346 publications

References 24 publications

New particle formation and growth from methanesulfonic acid, trimethylamine and water

New particle formation and growth from methanesulfonic acid, trimethylamine and water

A Chemical Ionization Mass Spectrometer for ambient measurements of Ammonia

Open-path, quantum cascade-laser-based sensor for high-resolution atmospheric ammonia measurements

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