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Book ; Online: An estimation of the 18O / 16O ratio of UT/LMS ozone based on artefact CO in air sampled during CARIBIC flights

Gromov, S. / Brenninkmeijer, C. A. M.

eISSN: 1680-7324

2015

Abstract: An issue of O 3 -driven artefact production of O 3 in the upper troposphere/lowermost stratosphere (UT/LMS) air analysed in the CARIBIC-1 project is being discussed. By confronting the CO mixing and isotope ratios obtained from different analytical ... ...

Abstract	An issue of O 3 -driven artefact production of O 3 in the upper troposphere/lowermost stratosphere (UT/LMS) air analysed in the CARIBIC-1 project is being discussed. By confronting the CO mixing and isotope ratios obtained from different analytical instrumentation, we (i) reject natural/artificial sampling and mixing effects as possible culprits of the problem, (ii) ascertain the chemical nature and quantify the strength of the contamination, and (iii) demonstrate successful application of the isotope mass-balance calculations for inferring the isotope composition of the contamination source. The δ 18 O values of the latter indicate that the oxygen is very likely being inherited from O 3 . The δ 13 C values hint at reactions of trace amounts of organics with stratospheric O 3 that could have yielded the artificial CO. While the exact contamination mechanism is not known, it is clear that the issue pertains only to the earlier (first) phase of the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) project. Finally, estimated UT/LMS ozone δ 18 O values are lower than those observed in the stratosphere within the same temperature range, suggesting that higher pressures (240–270 hPa) imply lower isotope fractionation controlling the local δ 18 O(O 3 ) value.
Subject code	333 ; 290
Language	English
Publishing date	2015-02-24
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Article ; Online: Applications of stable isotope analysis to atmospheric trace gas budgets

Brenninkmeijer C. A.M.

EPJ Web of Conferences, Vol 1, Pp 137-

2009 Volume 148

Abstract: Stable isotope analysis has become established as a useful method for tracing the budgets of atmospheric trace gases and even atmospheric oxygen. Several new developments are briefly discussed in a systematic way to give a practical guide to the scope of ...

Abstract	Stable isotope analysis has become established as a useful method for tracing the budgets of atmospheric trace gases and even atmospheric oxygen. Several new developments are briefly discussed in a systematic way to give a practical guide to the scope of recent work. Emphasis is on applications and not on instrumental developments. Processes and reactions are less considered than applications to resolve trace gas budgets. Several new developments are promising and applications hitherto not considered to be possible may allow new uses.
Keywords	Physics ; QC1-999 ; Science ; Q ; DOAJ:Physics (General) ; DOAJ:Physics and Astronomy
Language	English
Publishing date	2009-02-01T00:00:00Z
Publisher	EDP Sciences
Document type	Article ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book: Repräsentative, mittelfristige Beobachtungen von Spurengasen und Aerosolen in der oberen Troposphäre und unteren Stratosphäre (OT/US) mit CARIBIC

Brenninkmeijer, C. A. M

Abschlussbericht zum BMBF-Vorhaben ; [Laufzeit: 01.04.2001 - 31.03.2004]

2004

Institution	Max-Planck-Institut für Chemie
Author's details	Max-Planck-Institut für Chemie. C. A. M. Brenninkmeijer
Language	German
Size	32, 4 Bl., Ill., graph. Darst.
Publishing place	Mainz
Document type	Book
Note	Förderkennzeichen BMBF 07 ATF 15. - Literaturangaben ; Unterschiede zwischen dem gedruckten Dokument und der elektronischen Ressource können nicht ausgeschlossen werden
Database	Library catalogue of the German National Library of Science and Technology (TIB), Hannover

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Book ; Online: Repräsentative, mittelfristige Beobachtungen von Spurengasen und Aerosolen in der oberen Troposphäre und unteren Stratosphäre (OT/US) mit CARIBIC

Brenninkmeijer, C. A. M

Abschlußbericht zum BMBF-Vorhaben ; [Laufzeit: 01.04.2001 - 31.03.2004]

2004

Institution	Max-Planck-Institut für Chemie
Author's details	Max-Planck-Institut für Chemie. C. A. M. Brenninkmeijer
Language	German
Size	Online-Ressource (31 S., 1,57 MB), Ill., graph. Darst.
Publisher	Technische Informationsbibliothek u. Universitätsbibliothek
Publishing place	Hannover ; Mainz
Document type	Book ; Online
Note	Förderkennzeichen BMBF 07ATF15. - Literaturverz. ; IMD-Felder maschinell generiert ; Unterschiede zwischen der gedruckten und der elektronischen Dokumentversion sind möglich
Database	Library catalogue of the German National Library of Science and Technology (TIB), Hannover

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Article: N₂O as a tracer of mixing stratospheric and tropospheric air based on CARIBIC data with applications for CO₂

Assonov, S.S / Brenninkmeijer, C.A.M / Schuck, T / Umezawa, T

Atmospheric environment. 2013 Nov., v. 79

2013

Abstract: Stratosphere–troposphere exchange (STE) affects distributions of trace gases, with ozone (O₃) and CO being commonly used to study mixing process in the UTLS (Upper Troposphere and Lower Stratosphere) region. Here we explore the application of N₂O as a ... ...

Abstract	Stratosphere–troposphere exchange (STE) affects distributions of trace gases, with ozone (O₃) and CO being commonly used to study mixing process in the UTLS (Upper Troposphere and Lower Stratosphere) region. Here we explore the application of N₂O as a tracer of stratosphere to troposphere flux for CO₂ and its isotopes, using N₂O and CO₂ mixing ratios including a set of CO₂ isotope data for CARIBIC aircraft samples and NOAA-Carbon Cycle flask samples. A frequency distribution of CARIBIC N₂O data (mostly UTLS at mid- and high-latitudes) reveals a narrow distribution around a tropospheric maximum at nearly the same N₂O mixing ratio as the distribution peak for the station Mauna Loa (MLO) however with a skewing due to STE. We demonstrate that upper-tropospheric and STE-affected air can be distinguished using a threshold value based on the N₂O distribution width at MLO. A comparison with the use of O₃ is given. N₂O is discussed to be a robust and linear (season and latitude independent) tracer of STE mixing proportions. We propose that CARIBIC data coupled with CO₂ isotopic data published for the stratosphere and data of NOAA stations can be used as a frame of reference for δ¹⁸O(CO₂) and Δ¹⁷O(CO₂) STE fluxes. The Δ¹⁷O(CO₂) flux is of particular interest as it is thought to constrain estimates of biosphere productivity, atmospheric oxygen cycle and global gross CO₂ fluxes. CARBIC data can also help tracing STE flux by deep stratospheric intrusions and a data analysis is given for the Walliguan (WLG) observatory on the Tibetan Plateau.
Keywords	air ; aircraft ; atmospheric chemistry ; biosphere ; carbon dioxide ; isotopes ; latitude ; mixing ; nitrous oxide ; oxygen ; ozone ; stratosphere ; troposphere ; China
Language	English
Dates of publication	2013-11
Size	p. 769-779.
Publishing place	Elsevier Ltd
Document type	Article
ZDB-ID	216368-8
ISSN	0004-6981 ; 1352-2310
ISSN	0004-6981 ; 1352-2310
DOI	10.1016/j.atmosenv.2013.07.035
Database	NAL-Catalogue (AGRICOLA)

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Article: A system for high-quality CO2 isotope analyses of air samples collected by the CARIBIC Airbus A340-600.

Assonov, S / Taylor, P / Brenninkmeijer, C A M

Rapid communications in mass spectrometry : RCM

2009 Volume 23, Issue 9, Page(s) 1347–1363

Abstract: In 2007, JRC-IRMM began a series of atmospheric CO2 isotope measurements, with the focus on understanding instrumental effects, corrections as well as metrological aspects. The calibration approach at JRC-IRMM is based on use of a plain CO2 sample ( ... ...

Abstract	In 2007, JRC-IRMM began a series of atmospheric CO2 isotope measurements, with the focus on understanding instrumental effects, corrections as well as metrological aspects. The calibration approach at JRC-IRMM is based on use of a plain CO2 sample (working reference CO2) as a calibration carrier and CO2-air mixtures (in high-pressure cylinders) to determine the method-related correction under actual analytical conditions (another calibration carrier, in the same form as the samples). Although this approach differs from that in other laboratories, it does give a direct link to the primary reference NBS-19-CO2. It also helps to investigate the magnitude and nature for each of the instrumental corrections and allows for the quantification of the uncertainty introduced. Critical tests were focused on the instrumental corrections. It was confirmed that the use of non-symmetrical capillary crimping (an approach used here to deal with small samples) systematically modifies delta13C(CO2) and delta18O(CO2), with a clear dependence on the amount of extracted CO2. However, the calibration of CO2-air mixtures required the use of the symmetrical dual-inlet mode. As a proof of our approach, we found that delta13C(CO2) on extracts from mixtures agreed (within 0.010 per thousand) with values obtained from the 'mother' CO2 used for the mixtures. It was further found that very low levels of hydrocarbons in the pumping systems and the isotope ratio mass spectrometry (IRMS) instrument itself were critical. The m/z 46 values (consequently the calculated delta18O(CO2) values) are affected by several other effects with traces of air co-trapped with frozen CO2 being the most critical. A careful cryo-distillation of the extracted CO2 is recommended. After extensive testing, optimisation, and routine automated use, the system was found to give precise data on air samples that can be traced with confidence to the primary standards. The typical total combined uncertainty in delta13C(CO2) and delta18O(CO2) on the VPDB-CO2 scale, estimated on runs of CO2-air mixtures, is +/-0.040 per thousand and 0.060 per thousand (2-sigma values). Inter-comparison with MPI-BGC resulted in a scale discrepancy of a similar magnitude. Although the reason(s) for this discrepancy still need to be understood, this basically confirms the approach of using specifically prepared CO2-air mixtures as a calibration carrier, in order to achieve scale unification among laboratories. As important practical application and as a critical test, JRC-IRMM took part in the passenger aircraft-based global monitoring project CARIBIC (http://www.caribic-atmospheric.com). In this way, reliable CO2 isotope data for the tropopause region and the free troposphere were obtained. From June 2007 to January 2009, approximately 500 CARIBIC air samples have been analysed. Some flights demonstrated a compact correlation of both delta13C(CO2) and delta18O(CO2) with respect to CO2 concentration, demonstrating mixing of tropospheric and stratospheric air masses. These excellent correlations provide an independent, realistic data quality check.
MeSH term(s)	Air/analysis ; Air/standards ; Calibration/standards ; Carbon Dioxide/analysis ; Carbon Dioxide/standards ; Carbon Isotopes/analysis ; Carbon Isotopes/standards ; Europe ; Mass Spectrometry/instrumentation ; Mass Spectrometry/methods ; Mass Spectrometry/standards ; Oxygen Isotopes/analysis ; Oxygen Isotopes/standards ; Reference Values ; Research Design/standards
Chemical Substances	Carbon Isotopes ; Oxygen Isotopes ; Carbon Dioxide (142M471B3J)
Language	English
Publishing date	2009-05
Publishing country	England
Document type	Journal Article
ZDB-ID	58731-x
ISSN	1097-0231 ; 0951-4198
ISSN (online)	1097-0231
ISSN	0951-4198
DOI	10.1002/rcm.4008
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Article: CO2 isotope analyses using large air samples collected on intercontinental flights by the CARIBIC Boeing 767.

Assonov, S S / Brenninkmeijer, C A M / Koeppel, C / Röckmann, T

Rapid communications in mass spectrometry : RCM

2009 Volume 23, Issue 6, Page(s) 822–830

Abstract: Analytical details for 13C and 18O isotope analyses of atmospheric CO2 in large air samples are given. The large air samples of nominally 300 L were collected during the passenger aircraft-based atmospheric chemistry research project CARIBIC and analyzed ...

Abstract	Analytical details for 13C and 18O isotope analyses of atmospheric CO2 in large air samples are given. The large air samples of nominally 300 L were collected during the passenger aircraft-based atmospheric chemistry research project CARIBIC and analyzed for a large number of trace gases and isotopic composition. In the laboratory, an ultra-pure and high efficiency extraction system and high-quality isotope ratio mass spectrometry were used. Because direct comparison with other laboratories was practically impossible, the extraction and measurement procedures were tested in considerable detail. Extracted CO2 was measured twice vs. two different working reference CO2 gases of different isotopic composition. The two data sets agree well and their distributions can be used to evaluate analytical errors due to isotope measurement, ion corrections, internal calibration consistency, etc. The calibration itself is based on NBS-19 and also verified using isotope analyses on pure CO2 gases (NIST Reference Materials (RMs) and NARCIS CO2 gases). The major problem encountered could be attributed to CO2-water exchange in the air sampling cylinders. This exchange decreased over the years. To exclude artefacts due to such isotopic exchange, the data were filtered to reject negative delta18O(CO2) values. Examples of the results are given.
Language	English
Publishing date	2009-03
Publishing country	England
Document type	Journal Article
ZDB-ID	58731-x
ISSN	1097-0231 ; 0951-4198
ISSN (online)	1097-0231
ISSN	0951-4198
DOI	10.1002/rcm.3946
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Article: On the N2O correction used for mass spectrometric analysis of atmospheric CO2.

Assonov, S S / Brenninkmeijer, C A M

Rapid communications in mass spectrometry : RCM

2006 Volume 20, Issue 11, Page(s) 1809–1819

Abstract: To obtain accurate values of delta(13)C(CO(2)) and delta(18)O(CO(2)) on environmental CO(2) by mass spectrometry, the raw isotope data must be corrected for the isobaric N(2)O contribution. This is one of the analytical problems limiting inter-laboratory ...

Abstract	To obtain accurate values of delta(13)C(CO(2)) and delta(18)O(CO(2)) on environmental CO(2) by mass spectrometry, the raw isotope data must be corrected for the isobaric N(2)O contribution. This is one of the analytical problems limiting inter-laboratory delta(13)C(CO(2)) data consistency. The key parameter, the N(2)O relative ionisation efficiency (E(N2O)), cannot be determined with sufficient accuracy by direct measurements of pure N(2)O. The determination of (E(N2O)) by analyses on N(2)O--CO(2) mixtures of known isotope composition and mixing proportions has been recently suggested. In this work we propose a new method of N(2)O correction which uses the m/z 30 signal as a measure of the N(2)O/CO(2) ratio, so that determinations of (E(N2O)) and N(2)O content are not required. The method uses the fact that fragment-ion spectra of N(2)O and CO(2) are very specific. The formalism of the correction is considered. Various tests demonstrate that the new method is robust, stable and easy to implement in practice. The effective value (E(N2O)) (the key parameter for the new correction) has to be calibrated on known N(2)O--CO(2) mixtures by measuring (30)R signals only. The method accuracy we presently achieved is around 2.5% and any error which appears to come mostly from our N(2)O--CO(2) mixture preparation. Based on our tests and error considerations, the error of the proposed method that may be achieved is as low as +/-1.5% (relative to the correction magnitude). For tropospheric CO(2) this means +/-0.003 per thousand and +/-0.005 per thousand for delta(13)C(CO(2)) and delta(18)O(CO(2)), respectively. The proposed method may be valuable for small samples where no separate N(2)O determinations are available (e.g. ice core samples and CF-IRMS measurements) as well as for determination of (E(N2O)) and testing the 'traditional' N(2)O correction based on mass balance calculations.
Language	English
Publishing date	2006
Publishing country	England
Document type	Journal Article
ZDB-ID	58731-x
ISSN	1097-0231 ; 0951-4198
ISSN (online)	1097-0231
ISSN	0951-4198
DOI	10.1002/rcm.2516
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Article: Reporting small Delta 17O values: existing definitions and concepts.

Assonov, S S / Brenninkmeijer, C A M

Rapid communications in mass spectrometry : RCM

2005 Volume 19, Issue 5, Page(s) 627–636

Abstract: The three-isotope tracer Delta(17)O is increasingly used in atmospheric chemistry and other research areas. Thanks to the development of isotope-ratio mass spectrometry (IRMS), delta(17)O and delta(18)O can be determined with a precision of a few 0.01 ... ...

Abstract	The three-isotope tracer Delta(17)O is increasingly used in atmospheric chemistry and other research areas. Thanks to the development of isotope-ratio mass spectrometry (IRMS), delta(17)O and delta(18)O can be determined with a precision of a few 0.01 per thousand, and values for Delta(17)O may be calculated with similar precision. However, interpreting small and precisely determined Delta(17)O values as a deviation from an expected mass-dependent fractionation process is not straightforward. Several aspects are of high importance. In the present paper we review existing definitions, formulas and some other aspects of Delta(17)O reporting. One of the most confusing aspects is a variance of definitions and corresponding formulas. While Delta(17)O is traditionally defined to characterise a data point, i.e. Delta(17)O is considered as a deviation from an expected mass-fractionation line, the recently introduced definition (Miller MF. Geochim. Cosmochim. Acta 2002; 66: 188) characterises a fractionation line itself, in terms of its ordinate intercept. The formulas corresponding to this definition gives a characteristic for a specific process. When the 'traditionally defined' Delta(17)O is in use, an expected fractionation processes--the key point for Delta(17)O reporting--should be defined and parameterised with the same accuracy as intended for reporting Delta(17)O. When Delta(17)O is reported for a data point, not only a value for lambda but an ordinate intercept of a reference fractionation line should be given with high accuracy. We note that defining a single fractionation process is hardly possible for many natural compounds. For such compounds we propose to use a phenomenological reference line, namely an isotope composition range of natural sources. Next, aspects of Delta(17)O comparison and mass-balance calculations are considered. All the aspects considered for Delta(17)O may be relevant for others three-isotope tracers, e.g. Delta(33)S.
MeSH term(s)	Algorithms ; Computer Simulation ; Germany ; Guidelines as Topic ; Mass Spectrometry/methods ; Mass Spectrometry/standards ; Models, Chemical ; Oxygen Compounds/analysis ; Oxygen Compounds/chemistry ; Oxygen Isotopes/analysis ; Oxygen Isotopes/chemistry ; Oxygen Isotopes/standards ; Reference Values ; Reproducibility of Results ; Sensitivity and Specificity
Chemical Substances	Oxygen Compounds ; Oxygen Isotopes
Language	English
Publishing date	2005
Publishing country	England
Document type	Evaluation Studies ; Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	58731-x
ISSN	1097-0231 ; 0951-4198
ISSN (online)	1097-0231
ISSN	0951-4198
DOI	10.1002/rcm.1833
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Book: Development and Application of the 14CO Methodology for Validating OH Distribution, Incorporating a Stable Study of Europe s CO Budget

Brenninkmeijer, C.A.M.

Abstract: Knowledge about distribution and seasonality of the pivotal atmospheric oxidant hydroxyl (OH) is essential to understand tropospheric chemistry, the distribution of reactive trace gases and their rates of removal from the atmosphere. A new and promising ... ...

Title variant	Entwicklung und Anwendung des C-14-Verfahrens fuer die Validierung der OH-Verteilung unter Einbeziehung einer stabilen Studie zum CO-Haushalt Europas
Institution	Max-Planck-Gesellschaft zur Foerderung der Wissenschaften, Max-Planck-Institut fuer Chemie, 55020, 55020, Mainz, DE
Abstract	Knowledge about distribution and seasonality of the pivotal atmospheric oxidant hydroxyl (OH) is essential to understand tropospheric chemistry, the distribution of reactive trace gases and their rates of removal from the atmosphere. A new and promising methodology for determining OH distribution is emerging. This new method is based on the detection of 14CO in the atmosphere. 14CO is a direct consequence of the interaction of cosmic radiation with the earth s atmosphere. Most neutrons produced eventually lead to 14CO via the nuclear reaction 14N(n,p) 14C. The freshly formed 14C is very rapidly oxidized to 14CO. It is the subsequent step of 14CO+OH = 14CO2+H which allows the assessment of OH, because 14CO production is known and resulting 14CO levels can be measured. Thanks to the recent advances in accelerator mass spectrometry (AMS) the extremely rare 14CO can be detected accurately. It is intended to determine 14CO bimonthly at 5 continental locations for 2 1/2 years starting at the upcoming solar minimum of solar cycle number 22. One additional very important site will be the GAW station of Izasa, Canary Islands (Spain), being more representative for the remote atmosphere, and lower latitudes. Two experiments are to be integral part of this project. One utilizes an elegant very recent development for direct measurement of the actual in situ production of 14CO by cosmic radiation. In this way the source and its modulation are better defined. The other experiment is the development of a time integrating alternative measurement technique. The project will give considerable details about CO in Europe, because next to concentration measurements, the 13C and 18O stable isotopic composition will be known as well. Analysis of these data will allow in a unique, and hitherto for Europe new way to constrain source estimates based on the isotopic partitioning. A major effort also will be directed in 3D modelling for studying the actual success of models to reproduce the various aspects of the new 14CO data. Presently, models have performed poorly in explaining 14CO data, which is due to some fundamental new challenging aspects of 14CO as compared to the usual test species, mainly methylchloroform (CH3CC13). Models transport properties as well as their OH distribution will be evaluated and improved, ultimately leading to a better understanding of the rate of removal of pollutants, with emphasis on Europe.
Keywords	Oxidationsmittel ; In-Situ ; Hydroxid ; Radikal ; Kohlenmonoxid ; Troposphaere ; Chemie ; Messstation ; Massenspektrometrie ; Chemische Reaktion ; Isotop ; Konzentrationsmessung ; Messtechnik ; Stoffbilanz ; Europa
Language	English
Document type	Book
Remark	project start: 01/01/1997 project end: 12/31/1999 grant ID: ENV4-CT96-0318
Database	Environmental research database (UFORDAT) of the German Federal Environment Agency (UBA)

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