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Book ; Online: A Versatile Vacuum Ultraviolet Ion Source for Reduced Pressure Bipolar Chemical Ionization Mass Spectrometry

Breitenlechner, Martin / Novak, Gordon A. / Neuman, J. Andrew / Rollins, Andrew W. / Veres, Patrick R.

eISSN: 1867-8548

2021

Abstract: We present the development of a Chemical Ionization Mass Spectrometer (CIMS) ion source specifically designed for in situ measurements of trace gases in the upper troposphere and lower stratosphere. The ion source utilizes a commercially available ... ...

Abstract	We present the development of a Chemical Ionization Mass Spectrometer (CIMS) ion source specifically designed for in situ measurements of trace gases in the upper troposphere and lower stratosphere. The ion source utilizes a commercially available photoionization krypton lamp, primarily emitting photons in the vacuum ultraviolet (VUV) region at wavelengths of 124 and 117 nm (corresponding to energies of 10 and 10.6 eV, respectively), coupled to a commercially available Vocus Proton Transfer Reaction Mass Spectrometer. The VUV ion source can produce both negative and positive reagent ions, however, here we primarily focus on generating iodide anions (I − ). The instrument’s drift tube (also known as ion molecule reactor) operates at pressures between 2 and 10 mbar, which facilitates ambient sampling at atmospheric pressures as low as 50 mbar. The low operating pressure reduces secondary ion chemistry that can occur in iodide CIMS. It also allows the addition of water vapor to the drift tube to exceed typical ambient humidity by more than one order of magnitude, significantly reducing ambient humidity dependence of sensitivities. An additional benefit of this ion source and drift tube is a 10 to 100-fold reduction in nitrogen consumed during operation relative to standard I − ion sources, resulting in significantly reduced instrument weight and operational costs. In iodide mode, sensitivities of 76 cps/ppt for nitric acid, 35 cps/ppt for Br 2 , and 8.9 cps/ppt for Cl 2 were achieved. Lastly, we demonstrate that this ion source can generate benzene (C 6 H 6 + ) and ammonium (NH 4 + ) reagent ions to expand the number of detected atmospheric trace gases.
Subject code	333
Language	English
Publishing date	2021-10-14
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Article: PTR3: An Instrument for Studying the Lifecycle of Reactive Organic Carbon in the Atmosphere

Breitenlechner, Martin / Curtius Joachim / Fischer Lukas / Hainer Markus / Hansel Armin / Heinritzi Martin

Analytical chemistry. 2017 June 06, v. 89, no. 11

2017

Abstract: We have developed and characterized the novel PTR3, a proton transfer reaction-time-of-flight mass spectrometer (PTR-TOF) using a new gas inlet and an innovative reaction chamber design. The reaction chamber consists of a tripole operated with rf ... ...

Abstract	We have developed and characterized the novel PTR3, a proton transfer reaction-time-of-flight mass spectrometer (PTR-TOF) using a new gas inlet and an innovative reaction chamber design. The reaction chamber consists of a tripole operated with rf voltages generating an electric field only in the radial direction. An elevated electrical field is necessary to reduce clustering of primary hydronium (HâOâº) and product ions with water molecules present in the sample gas. The axial movement of the ions is achieved by the sample gas flow only. Therefore, the new design allows a 30-fold longer reaction time and a 40-fold increase in pressure compared to standard PTR-TOF-MS. First calibration tests show sensitivities of up to 18000 counts per second/parts per billion and volume (cps/ppbv) at a mass resolution of >8000 m/Îm (fwhm). The new inlet using center-sampling through a critical orifice reduces wall losses of low volatility compounds. Therefore, the new PTR3 instrument is sensitive to VOC typically present in the ppbv range as well as to semivolatile organic compounds (SVOC) and even highly oxidized organic molecules (HOMs) present in the parts per quadrillion per volume (ppqv) range in the atmosphere.
Keywords	carbon ; electric field ; electric power ; ions ; spectrometers ; volatile organic compounds
Language	English
Dates of publication	2017-0606
Size	p. 5824-5831.
Publishing place	American Chemical Society
Document type	Article
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021%2Facs.analchem.6b05110
Database	NAL-Catalogue (AGRICOLA)

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Article: Using collision-induced dissociation to constrain sensitivity of ammonia chemical ionization mass spectrometry (

Zaytsev, Alexander / Breitenlechner, Martin / Koss, Abigail R / Lim, Christopher Y / Rowe, James C / Kroll, Jesse H / Keutsch, Frank N

Atmospheric measurement techniques

2019 Volume 12, Issue 3, Page(s) 1861–1870

Abstract: Chemical ionization mass spectrometry (CIMS) instruments routinely detect hundreds of oxidized organic compounds in the atmosphere. A major limitation of these instruments is the uncertainty in their sensitivity to many of the detected ions. We describe ... ...

Abstract	Chemical ionization mass spectrometry (CIMS) instruments routinely detect hundreds of oxidized organic compounds in the atmosphere. A major limitation of these instruments is the uncertainty in their sensitivity to many of the detected ions. We describe the development of a new high-resolution time-of-flight chemical ionization mass spectrometer that operates in one of two ionization modes: using either ammonium ion ligand-switching reactions such as for
Language	English
Publishing date	2019-03-20
Publishing country	Germany
Document type	Journal Article
ZDB-ID	2505596-3
ISSN	1867-8548 ; 1867-1381
ISSN (online)	1867-8548
ISSN	1867-1381
DOI	10.5194/amt-12-1861-2019
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Article ; Online: PTR3: An Instrument for Studying the Lifecycle of Reactive Organic Carbon in the Atmosphere.

Breitenlechner, Martin / Fischer, Lukas / Hainer, Markus / Heinritzi, Martin / Curtius, Joachim / Hansel, Armin

Analytical chemistry

2017 Volume 89, Issue 11, Page(s) 5824–5831

Abstract	We have developed and characterized the novel PTR3, a proton transfer reaction-time-of-flight mass spectrometer (PTR-TOF) using a new gas inlet and an innovative reaction chamber design. The reaction chamber consists of a tripole operated with rf voltages generating an electric field only in the radial direction. An elevated electrical field is necessary to reduce clustering of primary hydronium (H
Language	English
Publishing date	2017-05-11
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021/acs.analchem.6b05110
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Book ; Online: Application of chemical derivatization techniques combined with chemical ionization mass spectrometry to detect stabilized Criegee intermediates and peroxy radicals in the gas phase

Zaytsev, Alexander / Breitenlechner, Martin / Novelli, Anna / Fuchs, Hendrik / Knopf, Daniel A. / Kroll, Jesse H. / Keutsch, Frank N.

eISSN: 1867-8548

2021

Abstract: Short-lived highly reactive atmospheric species, such as organic peroxy radicals ( RO 2 ) and stabilized Criegee intermediates (SCIs), play an important role in controlling the oxidative removal and transformation of many natural and anthropogenic trace ... ...

Abstract	Short-lived highly reactive atmospheric species, such as organic peroxy radicals ( RO 2 ) and stabilized Criegee intermediates (SCIs), play an important role in controlling the oxidative removal and transformation of many natural and anthropogenic trace gases in the atmosphere. Direct speciated measurements of these components are extremely helpful for understanding their atmospheric fate and impact. We describe the development of an online method for measurements of SCIs and RO 2 in laboratory experiments using chemical derivatization and spin trapping techniques combined with H 3 O + and <math xmlns="http://www.w3.org/1998/Math/MathML" id="M4" display="inline" overflow="scroll" dspmath="mathml"><mrow class="chem"><msubsup><mi mathvariant="normal">NH</mi><mn mathvariant="normal">4</mn><mo>+</mo></msubsup></mrow></math> <svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="24pt" height="15pt" class="svg-formula" dspmath="mathimg" md5hash="dd01b19a584d9ff35339d41174090f98"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="amt-14-2501-2021-ie00001.svg" width="24pt" height="15pt" src="amt-14-2501-2021-ie00001.png"/></svg:svg> chemical ionization mass spectrometry (CIMS). Using chemical derivatization agents with low proton affinity, such as electron-poor carbonyls, we scavenge all SCIs produced from a wide range of alkenes without depleting CIMS reagent ions. Comparison between our measurements and results from numeric modeling, using a modified version of the Master Chemical Mechanism, shows that the method can be used for the quantification of SCIs in laboratory experiments with a detection limit of 1.4×10 7 molecule cm −3 for an integration time of 30 s with the instrumentation used in this study. We show that spin traps are highly reactive towards atmospheric radicals and form stable adducts with them by studying the gas-phase kinetics of the reaction of spin traps with the hydroxyl radical (OH). We also demonstrate that spin trap adducts with SCIs and RO 2 can be simultaneously probed and quantified under laboratory conditions with a detection limit of 1.6×10 8 molecule cm −3 for an integration time of 30 s for RO 2 species with the instrumentation used in this study. Spin trapping prevents radical secondary reactions and cycling, ensuring that measurements are not biased by chemical interferences, and it can be implemented for detecting RO 2 species in laboratory studies and potentially in the ambient atmosphere.
Subject code	333
Language	English
Publishing date	2021-03-31
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book ; Online: Technical note

Bernhammer, Anne-Kathrin / Breitenlechner, Martin / Keutsch, Frank N. / Hansel, Armin

eISSN: 1680-7324

Conversion of isoprene hydroxy hydroperoxides (ISOPOOHs) on metal environmental simulation chamber walls

2017

Abstract: Sources and sinks of isoprene oxidation products from low-NO x isoprene chemistry have been studied at the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber with a custom-built selective reagent ion time-of-flight mass spectrometer (SRI-ToF-MS), ... ...

Abstract	Sources and sinks of isoprene oxidation products from low-NO x isoprene chemistry have been studied at the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber with a custom-built selective reagent ion time-of-flight mass spectrometer (SRI-ToF-MS), which allows quantitative measurement of isoprene hydroxy hydroperoxides (ISOPOOHs). The measured concentrations of the main oxidation products were compared to chemical box model simulations based on the Leeds Master Chemical Mechanism (MCM) v3.3. The modeled ISOPOOH concentrations are a factor of 20 higher than the observed concentrations, and methyl vinyl ketone (MVK) and methacrolein (MACR) concentrations are up to a factor of 2 lower compared to observations, despite the artifact-free detection method. Addition of catalytic conversion of 1,2-ISOPOOH and 4,3-ISOPOOH to methyl vinyl ketone (MVK) and methacrolein (MACR) on the stainless-steel surface of the chamber to the chemical mechanism resolves the discrepancy between model predictions and observation. This suggests that isoprene chemistry in a metal chamber under low-NO x conditions cannot be described by a pure gas phase model alone. Biases in the measurement of ISOPOOH, MVK, and MACR can be caused not only intra-instrumentally but also by the general experimental setup. The work described here extends the role of heterogeneous reactions affecting gas phase composition and properties from instrumental surfaces, described previously, to general experimental setups. The role of such conversion reactions on real environmental surfaces is yet to be explored.
Subject code	660 ; 540
Language	English
Publishing date	2017-03-24
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book ; Online: A Chemical Ionization Mass Spectrometry Utilizing Ammonium Ions (NH4+ CIMS) for Measurements of Organic Compounds in the Atmosphere

Xu, Lu / Coggon, Matthew M. / Stockwell, Chelsea E. / Gilman, Jessica B. / Robinson, Michael A. / Breitenlechner, Martin / Lamplugh, Aaron / Neuman, J. Andrew / Novak, Gordon A. / Veres, Patrick R. / Brown, Steven S. / Warneke, Carsten

eISSN: 1867-8548

2022

Abstract: In this study, we describe the characterization and field deployment of a Chemical Ionization Mass Spectrometry (CIMS) using a recently developed focusing ion-molecule reactor (FIMR) and ammonium-water cluster (NH 4 + ·H 2 O) as the reagent ion (denoted ... ...

Abstract	In this study, we describe the characterization and field deployment of a Chemical Ionization Mass Spectrometry (CIMS) using a recently developed focusing ion-molecule reactor (FIMR) and ammonium-water cluster (NH 4 + ·H 2 O) as the reagent ion (denoted as NH 4 + CIMS). We show that NH 4 + ·H 2 O is a highly versatile reagent ion for measurements of a wide range of oxygenated organic compounds. The major product ion is the cluster with NH 4 + produced via ligand-switching reactions. Other product ions (e.g., protonated ion, cluster ion with NH 4 + ·H 2 O, with H 3 O + , and with H 3 O + ·H 2 O) are also produced, but with minor fractions for most of the oxygenated compounds studied here. The instrument sensitivities (counts per second per ppbv, cps ppbv -1 ) and product distributions are strongly dependent on the instrument operating conditions, including the ratio of ammonia (NH 3 ) and H 2 O flows and the drift voltages, which should be carefully selected to ensure NH 4 + ·H 2 O as the predominant reagent ion and to optimize sensitivities. For monofunctional analytes, the NH 4 + ·H 2 O chemistry exhibits high sensitivity (i.e., > 1000 cps ppbv -1 ) towards ketones, moderate sensitivity (i.e., between 100 and 1000 cps ppbv -1 ) towards aldehdyes, alcohols, organic acids, and monoterpenes, low sensitivity (i.e., between 10 and 100 cps ppbv -1 ) towards isoprene and C1 and C2 organics, and negligible sensitivity (i.e., < 10 cps ppbv -1 ) towards reduced aromatics. The instrumental sensitivities of analytes depend on the binding energy of the analyte-NH 4 + cluster, which can be estimated using voltage scanning. This offers the possibility to constrain the sensitivity of analytes for which no calibration standards exist. This instrument was deployed in the RECAP campaign (Re-Evaluating the Chemistry of Air Pollutants in California) in Pasadena, California during summer 2021. Measurement comparisons against co-located mass spectrometers show that the NH 4 + CIMS is capable of detecting compounds from a wide ...
Subject code	333 ; 290
Language	English
Publishing date	2022-08-17
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Article: Dimensionality-reduction techniques for complex mass spectrometric datasets: application to laboratory atmospheric organic oxidation experiments.

Koss, Abigail R / Canagaratna, Manjula R / Zaytsev, Alexander / Krechmer, Jordan E / Breitenlechner, Martin / Nihill, Kevin J / Lim, Christopher Y / Rowe, James C / Roscioli, Joseph R / Keutsch, Frank N / Kroll, Jesse H

Atmospheric chemistry and physics

2020 Volume 20, Issue 2, Page(s) 1021–1041

Abstract: Oxidation of organic compounds in the atmosphere produces an immensely complex mixture of product species, posing a challenge for both their measurement in laboratory studies and their inclusion in air quality and climate models. Mass spectrometry ... ...

Abstract	Oxidation of organic compounds in the atmosphere produces an immensely complex mixture of product species, posing a challenge for both their measurement in laboratory studies and their inclusion in air quality and climate models. Mass spectrometry techniques can measure thousands of these species, giving insight into these chemical processes, but the datasets themselves are highly complex. Data reduction techniques that group compounds in a chemically and kinetically meaningful way provide a route to simplify the chemistry of these systems but have not been systematically investigated. Here we evaluate three approaches to reducing the dimensionality of oxidation systems measured in an environmental chamber: positive matrix factorization (PMF), hierarchical clustering analysis (HCA), and a parameterization to describe kinetics in terms of multigenerational chemistry (gamma kinetics parameterization, GKP). The evaluation is implemented by means of two datasets: synthetic data consisting of a three-generation oxidation system with known rate constants, generation numbers, and chemical pathways; and the measured products of OH-initiated oxidation of a substituted aromatic compound in a chamber experiment. We find that PMF accounts for changes in the average composition of all products during specific periods of time but does not sort compounds into generations or by another reproducible chemical process. HCA, on the other hand, can identify major groups of ions and patterns of behavior and maintains bulk chemical properties like carbon oxidation state that can be useful for modeling. The continuum of kinetic behavior observed in a typical chamber experiment can be parameterized by fitting species' time traces to the GKP, which approximates the chemistry as a linear, first-order kinetic system. The fitted parameters for each species are the number of reaction steps with OH needed to produce the species (the generation) and an effective kinetic rate constant that describes the formation and loss rates of the species. The thousands of species detected in a typical laboratory chamber experiment can be organized into a much smaller number (10-30) of groups, each of which has a characteristic chemical composition and kinetic behavior. This quantitative relationship between chemical and kinetic characteristics, and the significant reduction in the complexity of the system, provides an approach to understanding broad patterns of behavior in oxidation systems and could be exploited for mechanism development and atmospheric chemistry modeling.
Language	English
Publishing date	2020-01-27
Publishing country	Germany
Document type	Journal Article
ISSN	1680-7316
ISSN	1680-7316
DOI	10.5194/acp-20-1021-2020
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Book ; Online: Application of chemical derivatization techniques combined with chemical ionization mass spectrometry to detect stabilized Criegee intermediates and peroxy radicals in the gas phase

Zaytsev, Alexander / Breitenlechner, Martin / Novelli, Anna / Fuchs, Hendrik / Knopf, Daniel A. / Kroll, Jesse H. / Keutsch, Frank N.

eISSN: 1867-8548

2020

Abstract: Short-lived highly reactive atmospheric species, such as organic peroxy radicals (RO 2 ) and stabilized Criegee intermediates (SCIs), play an important role in controlling the oxidative removal and transformation of many natural and anthropogenic trace ... ...

Abstract	Short-lived highly reactive atmospheric species, such as organic peroxy radicals (RO 2 ) and stabilized Criegee intermediates (SCIs), play an important role in controlling the oxidative removal and transformation of many natural and anthropogenic trace gases in the atmosphere. Direct speciated measurements of these components are extremely helpful for understanding their atmospheric fate and impact. We describe the development of an online method for measurements of SCIs and RO 2 in laboratory experiments using chemical derivatization and spin trapping techniques combined with H 3 O + and NH 4 + chemical ionization mass spectrometry (CIMS). Using chemical derivatization agents with low proton affinity, such as electron-poor carbonyls, we scavenge all SCIs produced from a wide range of alkenes without depleting CIMS reagent ions. Comparison between our measurements and results from numeric modelling, using a modified version of the Master Chemical Mechanism, shows that the method can be used for quantification of SCIs in laboratory experiments with detection limit of 1.4 × 10 7 molecule cm -3 for 30 s integration time with the instrumentation used in this study. We show that spin traps are highly reactive towards atmospheric radicals and form stable adducts with them by studying the gas-phase kinetics of their reaction with hydroxyl radical (OH). We also demonstrate that spin trap adducts with SCIs and RO 2 can be simultaneously probed and quantified under laboratory conditions with detection limit of 1.6 × 10 8 molecule cm -3 for 30 s integration time for RO 2 species with the instrumentation used in this study. Spin trapping prevents radical secondary reactions and cycling, which ensures that measurements are not biased by chemical interferences, and can be implemented for detecting RO 2 species in the ambient atmosphere.
Subject code	333
Language	English
Publishing date	2020-09-30
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book ; Online: Technical Note

Bernhammer, Anne-Kathrin / Breitenlechner, Martin / Keutsch, Frank N. / Hansel, Armin / the CLOUD Team

eISSN: 1680-7324

Conversion of Isoprene Hydroxy Hydroperoxides (ISOPOOH) on Metal Environmental Simulation Chamber Walls

2016

Abstract: Sources and sinks of isoprene oxidation products from low NO x isoprene chemistry have been studied at the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber with a custom-built selective reagent ion time of flight mass spectrometer (SRI-ToF-MS), ... ...

Abstract	Sources and sinks of isoprene oxidation products from low NO x isoprene chemistry have been studied at the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber with a custom-built selective reagent ion time of flight mass spectrometer (SRI-ToF-MS), which allows quantitative measurement of isoprene hydroxy hydroperoxides (ISOPOOH). The measured concentrations of the main oxidation products were compared to chemical box model simulations based on the Leeds Master Chemical Mechanism (MCM) v3.3. The modelled ISOPOOH concentrations are by a factor of 20 higher than the observed and methyl vinyl ketone (MVK) and methacrolein (MACR) concentrations are by a factor of up to 2 lower compared to observations, despite the artifact-free detection method. Addition of catalytic conversion of 1,2-ISOPOOH and 4,3-ISOPOOH to MVK and MACR on the stainless steel surface of the chamber to the chemical mechanism resolves the discrepancy between model predictions and observation. This suggests that isoprene chemistry in a metal chamber under low NO x conditions cannot be described by a pure gas phase model alone. Biases in the measurement of ISOPOOH, MVK and MACR can not only be caused intra-instrumentally but also by the general experimental setup. The work described here extends the role of heterogeneous reactions affection gas phase composition and properties from instrumental surfaces, described previously, to general experimental setups. The role of such conversion reactions on real environmental surfaces is yet to be explored.
Subject code	660 ; 540
Language	English
Publishing date	2016-10-21
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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