Bisulfate – cluster based atmospheric pressure chemical ionization mass spectrometer for high-sensitivity (&amp;lt; 100 ppqV) detection of atmospheric dimethyl amine: proof-of-concept and first ambient data from boreal forest

Sipilä, Mikko; Sarnela, Nina; Jokinen, Tuija; Junninen, Heikki; Hakala, J.; Rissanen, Matti; Praplan, Arnaud P.; Simon, Mario; Kürten, Andreas; Bianchi, Federico; Dommen, Josef; Curtius, Joachim; Petäj̈ä, Tuukka; Worsnop, Douglas R.

doi:10.5194/amt-8-4001-2015

Cited by 40 publications

(40 citation statements)

References 29 publications

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“…Kieloaho et al (2013) found small alkylamines at levels of tens of parts per trillion by volume (ppt). Sipilä et al (2015) determined an upper limit for DMA of 0.15 ppt. The presence of as little as 5 ppt of DMA is enough to increase rates of NPF by about 6 orders of magnitude with respect to sulfuric acid and water alone (Almeida et al, 2013).…”

Section: Salt Formationmentioning

confidence: 99%

Evidence for Diverse Biogeochemical Drivers of Boreal Forest New Particle Formation

Lawler

Rissanen

Ehn

et al. 2018

Geophysical Research Letters

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New particle formation (NPF) is an important contributor to particle number in many locations, but the chemical drivers for this process are not well understood. Daytime NPF events occur regularly in the springtime Finnish boreal forest and strongly impact aerosol abundance. In April 2014 size‐resolved chemical measurements of ambient nanoparticles were made using the Time‐of‐Flight Thermal Desorption Chemical ionization Mass Spectrometer and we report results from two NPF events. While growth overall was dominated by terpene oxidation products, newly formed 20–70 nm particles showed enhancement in apparent alkanoic acids. The events occurred on days with rapid transport of marine air, which correlated with low background aerosol loading and higher gas phase methanesulfonic acid levels. These results are broadly consistent with previous studies on Nordic NPF but indicate that further attention should be given to the sources and role of non‐terpenoid organics and the possible contribution of transported marine compounds in this process.

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Section: Salt Formationmentioning

confidence: 99%

Evidence for Diverse Biogeochemical Drivers of Boreal Forest New Particle Formation

Lawler

Rissanen

Ehn

et al. 2018

Geophysical Research Letters

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“…Protonated ethanol or acetone ions were used as reagent ions by Yu and Lee (2012). Negative-ion detection of amines using bisulfate reagent ions has been described recently (Sipilä et al, 2015).…”

Section: Introductionmentioning

confidence: 99%

Detection of dimethylamine in the low pptv range using nitrate chemical ionization atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometry

et al. 2016

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Abstract. Amines are potentially important for atmospheric new particle formation, but their concentrations are usually low with typical mixing ratios in the pptv range or even smaller. Therefore, the demand for highly sensitive gas-phase amine measurements has emerged in the last several years. Nitrate chemical ionization mass spectrometry (CIMS) is routinely used for the measurement of gasphase sulfuric acid in the sub-pptv range. Furthermore, extremely low volatile organic compounds (ELVOCs) can be detected with a nitrate CIMS. In this study we demonstrate that a nitrate CIMS can also be used for the sensitive measurement of dimethylamine (DMA, (CH 3 ) 2 NH) using the NO − 3 q (HNO 3 ) 1−2 q (DMA) cluster ion signal. Calibration measurements were made at the CLOUD chamber during two different measurement campaigns. Good linearity between 0 and ∼ 120 pptv of DMA as well as a sub-pptv detection limit of 0.7 pptv for a 10 min integration time are demonstrated at 278 K and 38 % RH.

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“…In addition, novel in situ methods for measuring ambient air gas-phase amines have been developed, usually based on mass-spectrometric detection: chemical ionization mass spectrometry (CIMS), (Sellegri et al, 2005;You et al, 2014), ambient pressure proton transfer mass spectrometry (AmPMS) (Hanson et al, 2011;Freshour et al, 2014), chemical ionization atmospheric pressure interface time-of-flight mass spectrometry (CI-APi-TOF) Sipilä et al, 2015;Kürten et al, 2016), and TOF-CIMS (Zheng et al, 2015). These in situ techniques have short time resolution and the limits of detections are small.…”

Section: Introductionmentioning

confidence: 99%

Responce to Referee 2

Hemmilä¹

2018

Preprint

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We thank the Referee for very detailed and helpful comments, which we address in details below.1. There are far too many data tables and figures that are irrelevant to the structure of the results and discussion. Most can be replaced with a single sentence. These detract from the quality of the observations and should be relocated to a Supporting Information document. These are noted in detail below.Asked figures and tables were moved to Supporting Material.2. The Authors claim that they are reporting the longest time series of amines measurements to date, but the measurements are short-duration periods made in different C1 ACPD Interactive commentPrinter-friendly version Discussion paper months. A time series implies continuous data collection and the authors should revise the manuscript to be clear that they are reporting eight weeks of observations from different months over the course of a year from the same observation site. Further to this point, the sampling strategy reported and the findings discussed in the paper are all weakened because of the intermittent nature of these observations. The limitations of the dataset need to be presented clearly. Figure 7 is the only depiction of the full measurement time series and it appears that even within each observation period that there are gaps in the data which are not clearly explained. How can the Authors justify their conclusions regarding monthly/seasonal trends if they do not measure continuously throughout each?Number of data points in each month was added to Table 4. We also added clarification in Experimental section that due to instrumental problems good quality data was captured only 8 weeks, although we measured continuously. Even though measurements cover only 8 weeks, to our best knowledge, this is still largest data set of amine concentrations.3. The manuscript does not appear to have a clear purpose or objective. There are several discussions made throughout the manuscript that are not joined in a clear narrative, the final paragraph of the introduction for example, which confuses the meaning and scientific contribution of the findings.a. The Authors present an advancement in atmospheric amine measurement capabilities through the use of an ion chromatography-mass spectrometry system, but do not clearly demonstrate the necessary performance metrics (e.g. a sample chromatogram demonstrating the ability to speciate the suite of analytes likely to be encountered in the atmosphere). The data then presented in the tables and figures is still largely below the instrument detection limits (e.g. Table 4), so is this improvement really meeting the observational needs of the research community?We have added chromatogram to Supplement Material. It would be great to have better C2 ACPD Interactive commentPrinter-friendly version Discussion paper time resolution and lower detection limits, but this is the best which is possible at the moment. Direct mass spectrometric methods have lower detection limits and higher time resolution, but data is not species spec...

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Bisulfate – cluster based atmospheric pressure chemical ionization mass spectrometer for high-sensitivity (< 100 ppqV) detection of atmospheric dimethyl amine: proof-of-concept and first ambient data from boreal forest

Cited by 40 publications

References 29 publications

Evidence for Diverse Biogeochemical Drivers of Boreal Forest New Particle Formation

Evidence for Diverse Biogeochemical Drivers of Boreal Forest New Particle Formation

Detection of dimethylamine in the low pptv range using nitrate chemical ionization atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometry

Responce to Referee 2

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