New photolytic converter for improving aircraft measurements of NO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt; via chemiluminescence

Nussbaumer, Clara M.; Parchatka, Uwe; Tadić, Ivan; Bohn, Birger; Marno, Daniel; Martínez, Mònica; Rohloff, Roland; Harder, Hartwig; Kluge, Flora; Pfeilsticker, Klaus; Obersteiner, Florian; Zöger, Martin; Doerich, Raphael; Crowley, John N.; Lelieveld, Jos; Fischer, H.

doi:10.5194/amt-2021-180

Cited by 4 publications

(3 citation statements)

References 60 publications

(84 reference statements)

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“…The effect is transient and vanishes after a short time. The fact that rapidly changing water vapor concentrations can affect the instrumental background of CLS detectors and lead to a non-trivial memory effect that cannot be easily corrected retrospectively has also been reported recently in the literature (Nussbaumer et al 2021). (b) A small contamination of the milli-Q water and differences in the sample quality used for humidification cannot be fully ruled out.…”

Section: Figurementioning

confidence: 72%

Comparison of nitrous acid detection using open-path incoherent broadband cavity-enhanced absorption spectroscopy and extractive long-path absorption photometry

Dixneuf

Ruth

Häseler³

et al. 2021

Preprint

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Abstract. An instrument based on 20 m open-path incoherent broadband cavity-enhanced absorption spectroscopy (IBBCEAS) was established at the Jülich SAPHIR chamber in Spring 2011. The setup was optimized for the detection of HONO and NO2 in the near UV region 352–386 nm, utilizing a bright hot-spot Xe-arc lamp and a UV-enhanced CCD detector. A 2σ detection limit of 26 pptv for HONO and 76 pptv for NO2 was achieved for an integration time of 1 min. Methacrolein has also been detected at mixing ratios below 5 ppbv. The IBBCEAS instrument’s performance for HONO and NO2 detection was compared to that of extractive wet techniques, long-path absorption photometry (LOPAP) and chemiluminescence spectrometry (CLS) NOx detection, respectively.

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Section: Figurementioning

confidence: 72%

Comparison of nitrous acid detection using open-path incoherent broadband cavity-enhanced absorption spectroscopy and extractive long-path absorption photometry

Dixneuf

Ruth

Häseler³

et al. 2021

Preprint

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“…In addition, NO 2 was measured with a chemiluminescence (CLD) set-up (ECO PHYSICS; CLD 790 SR) equipped with a photolytic converter to convert NO 2 to NO (Tadic et al, 2020;Nussbaumer et al, 2021). This instrument also provided the campaign NO data set.…”

Section: No 3 Reactivitymentioning

confidence: 99%

Fate of the nitrate radical at the summit of a semi-rural mountain site in Germany assessed with direct reactivity measurements

Dewald¹,

Nussbaumer²,

Schuladen³

et al. 2022

Atmos. Chem. Phys.

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Abstract. The reactivity of NO3 plays an important role in modifying the fate of reactive nitrogen species at nighttime. High reactivity (e.g. towards unsaturated volatile organic compounds – VOCs) can lead to formation of organic nitrates and secondary organic aerosol, whereas low reactivity opens the possibility of heterogeneous NOx losses via the formation and uptake of N2O5 to particles. We present direct NO3 reactivity measurements (kNO3) that quantify the VOC-induced losses of NO3 during the TO2021 campaign at the summit of the Kleiner Feldberg mountain (825 m, Germany) in July 2021. kNO3 was on average ∼0.035 s−1 during the daytime, ∼0.015 s−1 for almost half of the nights and below the detection limit of 0.006 s−1 for the other half, which may be linked to sampling from above the nocturnal surface layer. NO3 reactivities derived from VOC measurements and the corresponding rate coefficient were in good agreement with kNO3, with monoterpenes representing 84 % of the total reactivity. The fractional contribution F of kNO3 to the overall NO3 loss rate (which includes an additional reaction of NO3 with NO and photolysis) were on average ∼16 % during the daytime and ∼50 %–60 % during the nighttime. The relatively low nighttime value of F is related to the presence of several tens of parts per trillion by volume (pptv) of NO on several nights. NO3 mixing ratios were not measured, but steady-state calculations resulted in nighttime values between <1 and 12 pptv. A comparison of results from TO2021 with direct measurements of NO3 during previous campaigns between 2008 and 2015 at this site revealed that NO3 loss rates were remarkably high during TO2021, while NO3 production rates were low. We observed NO mixing ratios of up to 80 pptv at night, which has implications for the cycling of reactive nitrogen at this site. With O3 present at levels of mostly 25 to 60 ppbv (parts per billion by volume), NO is oxidized to NO2 on a timescale of a few minutes. We find that maintaining NO mixing ratios of, e.g., 40 pptv requires a ground-level NO emission rate of 0.33 pptv s−1 (into a shallow surface layer of 10 m depth). This in turn requires a rapid deposition of NO2 to the surface (vdNO2∼0.15 cm s−1) to reduce nocturnal NO2 levels to match the observations.

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“…In addition, NO2 was measured with a chemiluminescence (CLD) setup (ECO Physics, CLD 790 SR) equipped with a photolytic converter to convert NO2 to NO (Tadic et al, 2020;Nussbaumer et al, 2021). This instrument also provided the campaign NO data-set.…”

Section: No2 No O3 and Actinic Fluxmentioning

confidence: 99%

Fate of the nitrate radical at the summit of a semi-rural mountain site in Germany assessed with direct reactivity measurements

Dewald

Nussbaumer

Schuladen

et al. 2022

Preprint

Self Cite

View full text Add to dashboard Cite

Abstract. The reactivity of NO3 plays an important role in modifying the fate of reactive nitrogen species at nighttime. High reactivity (e.g. towards unsaturated VOCs) can lead to formation of organic nitrates and secondary organic aerosol, whereas low reactivity opens the possibility of heterogeneous NOX losses via formation and uptake of N2O5 to particles. We present direct NO3 reactivity measurements (kNO3) that quantify the VOC-induced losses of NO3 during the TO2021 campaign at the summit of the Kleiner Feldberg mountain (825 m, Germany) in July 2021. kNO3 was on average ~ 0.035 s-1 during the daytime, ~ 0.015 s-1 for almost half of the nights and below the detection limit of 0.006 s-1 for the other half, which may be linked to sampling from above the nocturnal surface layer. NO3 reactivities derived from VOC measurements and the corresponding rate coefficient were in good agreement with kNO3, with monoterpenes representing 84 % of the total reactivity. The fractional contribution F of kNO3 to the overall NO3 loss rate (which includes additional reaction of NO3 with NO and photolysis) were on average ~16 % during the daytime and ~50–60 % during the nighttime. The relatively low nighttime value of F is related to the presence of several tens of pptv of NO on several nights. NO3 mixing ratios were not measured but steady-state calculations resulted in nighttime values between < 1 pptv and 12 pptv. A comparison of results from TO2021 with direct measurements of NO3 during previous campaigns between 2008 and 2015 at this site revealed that NO3 loss rates were remarkably high during TO2021, while NO3 production rates were low. We observed NO mixing ratios of up to 80 pptv at night which has implications for the cycling of reactive nitrogen at this site. With O3 present at levels of mostly 25 to 60 ppbv, NO is oxidised to NO2 on a time-scale of a few minutes. We find that to maintain NO mixing ratios of e.g. 40 pptv requires a ground-level NO emission rate of 0.33 pptv s-1 (into a shallow surface layer of 10 m depth). This in turn requires rapid deposition of NO2 to the surface (vdNO2 ~ 0.15 cm s-1) to reduce nocturnal NO2 levels to match the observations.

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New photolytic converter for improving aircraft measurements of NO<sub>2</sub> via chemiluminescence

Cited by 4 publications

References 60 publications

Comparison of nitrous acid detection using open-path incoherent broadband cavity-enhanced absorption spectroscopy and extractive long-path absorption photometry

Comparison of nitrous acid detection using open-path incoherent broadband cavity-enhanced absorption spectroscopy and extractive long-path absorption photometry

Fate of the nitrate radical at the summit of a semi-rural mountain site in Germany assessed with direct reactivity measurements

Fate of the nitrate radical at the summit of a semi-rural mountain site in Germany assessed with direct reactivity measurements

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