ONE-YEAR CLIMATOLOGY OF NITROGEN OXIDES AND OZONE IN THE TROPOPAUSE REGION RESULTS FROM B-747 AIRCRAFT MEASUREMENTS
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- Maja Lichtenberg
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1 Diss. ETH No ONE-YEAR CLIMATOLOGY OF NITROGEN OXIDES AND OZONE IN THE TROPOPAUSE REGION RESULTS FROM B-747 AIRCRAFT MEASUREMENTS A dissertation submitted to the SWISS FEDERAL INSTITUTE OF TECHNOLOGY (ETB) ZÜRICH for the degree of Doctor of Natural Seiences presented by DOMINIK WILHELM BRUNNER Dip!. Phys. ETH born 30 January 1967 citizen of Iseltwald (BE) accepted on the recommendation of Prof. Dr. A. Waldvogel, examiner Prof. Dr. U. Schumann, co-examiner Dr. J. Staehelin, co-examiner Zürich, 1998
2 ABSTRACT Ozone (0 3 ) is a chemically and radiatively important atmospheric trace gas. In the troposphere, 0 3 is formed from precursor substances such as nitrogen oxides (NO x ), volatile organic compounds (VOC) and carbon monoxide (CO), whieh all have important anthropogenie sources. Despite its role as a key component in trace gas chemistry, the distribution of tropospheric NO x is not well known. Particularly in the free troposphere which can not yet be reached by satellite instruments, the data coverage - mainly obtained by in-situ aircraft observations - is insufficient. This (PhD) thesis gives an overview of the NOXAR project (measurements of Nitrogen OXides and ozone along Air Routes) which intended to establish a representative data set of NO x and 0 3 measurements in the upper troposphere and the lower stratosphere over large parts of the northern hemisphere. To achieve this goal, a fully automated system for measuring 0 3, NO, and N0 2 was designed to operate during one year (May 1995 until May 1996) on a Swissair B-747 airliner. The analysers were installed together with all the auxiliary equipment (vacuum pumps, calibration deviee, electronic circuitry, etc.) in a purpose built rack designed to meet the stringent safety standards of civil aviation. The system was partially or fully operational during 4000 hrs on a total of 540 scheduled flights between Zurich and destinations in the USA and the Far East. The amount of data recorded by NOXAR represents approximately a tenfold increase over previous compilations of airborne NO x measurements in the altitude range 9-12 km. It covers for the first time large parts of the Asian continent and includes a full seasonal cycle. Detection limits of 23 pptv, 45 pptv and 500 pptv were achieved for 2-minute averages of NO, N0 2 and 0 3 respective1y. The sampled NO and 0 3 concentrations are in good agreement with comparable measurements performed in the framework of the European MOZAIC (Measurement of Ozone on Airbus In-Service Aircraft) and POLINAT (Pollution from Aircraft Emissions in the North Atlantic F1ight Corridor) programs. NO x and 03 concentrations were observed to be highly variable both in space and time. In mid-iatitudes, the cruising altitude of civil airliners is close to the tropopause. Because of variations in the tropopause altitude associated with high- and low pressure systems, 0 3 concentrations frequent1y "swap" between high stratospheric levels of typically 300 to 600 ppbv and low tropospheric va1ues of 40 to 150 ppbv during a flight. During the whole measuring period, about 2' 800 short NO x peaks and a few hundred broad plumes extending up to 2000 km along the flight track were observed. The short peaks are clearly attributable to the sampling in exv
3 haust plumes of other aircraft in the flight corridor. The broad plumes are believed to be caused by the combined effect of rapid upward transport of NO x from the poiluted continental boundary layer in thunderstorm clouds and by NO production in lightning strokes. These plumes are largely responsible for the high NO x concentrations observed in the upper troposphere over the continents in summer and to a smaller extent in other seasons as weil. The seasonal variation of NO x concentrations is therefore much more pronounced over North America and Europe than over the North Atlantic. Currently, several European and American research programs are studying the possible impact of present and future air traffic emissions on atmospheric ozone and climate. An important tool in these studies is the use of chemical transport- and general circulation models. Results from the models have to be validated by observations. Representative measurements of key chemical species as performed by NOXAR are particularly suited for this task. First results of comparisons indicate, that the difference between model calculated NO x concentrations and the NOXAR measurements can be as large as a factor of three. The extensive data set established in this work represents an important step forward towards a better understanding of the distribution of NO x at aircraft cruising altitudes and will help to narrow the large uncertainties which exist in current model simulations of the climatic impact of the rapidly increasing air traffic. VI
4 ZUSAMMENFASSUNG Ozon ist ein sowohl für die Atmosphärenchemie als auch für den Strahlungshaushalt der Erde und damit für das Klima wichtiges Spurengas. In der Troposphäre wird Ozon aus Vorläufersubstanzen wie den Stickoxiden, den flüchtigen Kohlenwasserstoffen sowie Kohlenmonoxid gebildet, deren Konzentrationen der Mensch entscheidend beeinflusst. Trotz ihrer wichtigen Rolle in der Spurenstoffchemie ist die Verteilung von Stickoxiden in der Troposphäre nur ungenügend bekannt. Grosse Wissenslücken bestehen insbesondere in der freien Troposphäre, wo keine Satellitenmessungen zur Verfügung stehen und bisher nur einige Dutzend episodische Flugzeugmessungen durchgeführt wurden. Im Projekt NOXAR (measurements of Nitrogen OXides and ozone along Air Routes) wurden ausgedehnte Messungen durchgeführt um ein möglichst repräsentatives Bild der Stickoxidverteilung in der oberen Troposphäre und der unteren Stratosphäre in der nördlichen Hemisphäre zu gewinnen. Dazu wurde ein vollautomatisches System zur Messung von NO, N0 2 und Ozon im Frachtraum eines Swissair Linienflugzeuges vom Typ B-747 untergebracht. Die Sensoren wurden mit den Zusatzkomponenten (Pumpen, Kalibrationseinheit, Steuerelektronik, etc.) in einem Rack montiert, das den strengen Sicherheitsbestimmungen genügte, die in der zivilen Luftfahrt angewendet werden. Zwischen Mai 1995 und Mai 1996 wurden auf 540 Flügen während insgesamt 4000 Stunden die chemischen Messgrössen zusammen mit meteorologischen Daten und Positionsangaben des Bordcomputers aufgezeichnet. Die Flüge verteilten sich auf drei Hauptrouten zwischen Zürich und Destinationen in den USA und in Fernost. Der Umfang des in dieser Arbeit erstellten Datensatzes bedeutet etwa eine Verzehnfachung gegenüber bisher vorliegenden NO x Messungen auf Reiseflughöhe (ca km ü. M.). Zum ersten Mal wurden zudem weite Gebiete des asiatischen Kontinents abgedeckt und ein homogener Datensatz erstellt, der sich über ein ganzes Jahr erstreckt. Es wurden Detektionslimiten von 23 pptv, 45 pptv und 500 pptv für 2-min Mittelwerte der Konzentrationen von NO, N0 2 und 0 3 erreicht. Die Messungen von NO und 0 3 stimmen gut mit vergleichbaren Messungen im Rahmen der Europäischen Forschungsprogramme MOZAIC (Measurement of Ozone on Airbus In-Service Aircraft) und POLINAT (Pollution from Aircraft Emissions in the North Atlantic Flight Corridor) überein. Die beobachteten Stickoxid- und Ozonkonzentrationen zeigen eine hohe zeitliche und räumliche Variabilität. In mittleren Breiten liegt die Reiseflughöhe etwa im Be- VB
5 reich der Tropopause. Variationen der Tropopausenhöhe unter dem Einfluss von Hoch- und Tiefdrucksystem bewirken, dass sich das Flugzeug abwechslungsweise in stratosphärischer Luft mit hohen Oj-Konzentrationen und in troposphärischer Luft mit vergleichsweise niedrigen Konzentrationen befindet. Während der einjährigen Messphase wurden mehrere tausend kurzzeitige Stickoxidspitzen und einige hundert ausgedehnte "Stickoxidwolken" beobachtet, die sich bis zu 2000 km entlang der Flugroute erstreckten. Die kurzzeitigen Erhöhungen sind auf das Durchqueren der Abgasfahnen voranfliegender Flugzeuge im Flugkorridor zurückzuführen. Die breiten Stickoxidwolken dagegen sind wahrscheinlich auf das Zusammenspiel zweier verschiedener Effekte zurückzuführen: auf den raschen Vertikaltransport von NOx aus der verschmutzten Grenzschicht in konvektiven Gewitterwolken und auf die Produktion von NO durch Blitzaktivität. Diese Erscheinungen tragen erheblich zu den beobachteten hohen Stickoxidkonzentrationen in der oberen Troposphäre über Nordamerika und Europa im Sommer bei und sind dafür verantwortlich, dass der saisonale Verlauf der Konzentrationen über den Kontinenten deutlich ausgeprägter ist als über dem Nordatlantik. Mehrere europäische und amerikanische Forschungsprogramme beschäftigen sich zur Zeit mit dem Einfluss der Stickoxidemissionen des heutigen und zukünftigen Flugverkehrs auf das atmosphärische Ozon und das Erdklirna. Eine wichtige Stütze dieser Studien sind Simulationen mit Chemie-Transport- und globalen Zirkulationsmodellen. Resultate dieser Modelle lassen sich am besten anhand repräsentativer Messungen beurteilen, wie sie in NOXAR durchgeführt wurden. Erste Vergleiche mit Modellsimulationen ergaben, dass die berechneten NOx-Felder um bis zu einem Faktor 3 von den Messungen abweichen. Die hier präsentierten Messungen stellen einen bedeutenden Schritt dar auf dem Weg zu einem besseren Verständnis der Verteilung von Stickoxiden auf Flughöhe und werden dazu beitragen, die noch erheblichen Unsicherheiten in Modellsimulationen bezüglich der Klimarelevanz des schnell wachsenden Flugverkehrs weiter einzuschränken. V111
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