Amplified Trace Gas Removal in the Troposphere

Hofzumahaus, A.; Rohrer, Franz; Lu, Keding; Bohn, Birger; Brauers, T.; Chang, Chih-Chung; Fuchs, Hendrik; Holland, F.; Kita, K.; Kondo, Yutaka; Li, Xin; Lou, Shengrong; Shao, Min; Zeng, Limin; Wahner, Andreas; Zhang, Yuanhang

doi:10.1126/science.1164566

Cited by 594 publications

(715 citation statements)

References 25 publications

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“…For example, Archibald et al [37] show that although comparison with OH is improved, HO 2 and the organic peroxy radical (RO 2 ) concentrations tend to increase to levels beyond the stated uncertainty of the measurements. This observation could provide some support for the argument of Hofzumahaus et al [40] and Whalley et al [41] of species able to act like NO and convert HO 2 to OH. However, to date no species have been identified as being able to propagate this chemistry at the rate required to reconcile measurements and modelling of HO x in these pristine environments.…”

Section: Local -Regional -Global Modellingsupporting

confidence: 77%

The impact of local surface changes in Borneo on atmospheric composition at wider spatial scales: coastal processes, land-use change and air quality

Pyle

Warwick

Harris

et al. 2011

Phil. Trans. R. Soc. B

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We present results from the OP3 campaign in Sabah during 2008 that allow us to study the impact of local emission changes over Borneo on atmospheric composition at the regional and wider scale. OP3 constituent data provide an important constraint on model performance. Treatment of boundary layer processes is highlighted as an important area of model uncertainty. Model studies of land-use change confirm earlier work, indicating that further changes to intensive oil palm agriculture in South East Asia, and the tropics in general, could have important impacts on air quality, with the biggest factor being the concomitant changes in NO x emissions. With the model scenarios used here, local increases in ozone of around 50 per cent could occur. We also report measurements of short-lived brominated compounds around Sabah suggesting that oceanic (and, especially, coastal) emission sources dominate locally. The concentration of bromine in short-lived halocarbons measured at the surface during OP3 amounted to about 7 ppt, setting an upper limit on the amount of these species that can reach the lower stratosphere.

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Section: Local -Regional -Global Modellingsupporting

confidence: 77%

The impact of local surface changes in Borneo on atmospheric composition at wider spatial scales: coastal processes, land-use change and air quality

Pyle

Warwick

Harris

et al. 2011

Phil. Trans. R. Soc. B

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“…These reactions constitute the first step in the process of photochemical O 3 production in the atmosphere. Total OH reactivity measurements in the urban atmosphere have been conducted in New York City, USA (Ren et al, 2003a(Ren et al, , 2003b, Mexico City, Mexico (Shirley et al, 2006), Mainz, Germany (Sinha et al, 2008), Pearl River Delta, China (Hofzumahaus et al, 2009;Lou et al, 2010), and Houston, USA (Mao et al, 2010). The values of the OH reactivity observed during these measurements vary widely, between 10 and 200 s À1 , which reflects considerable regional diversity in the urban atmosphere.…”

Section: Introductionmentioning

confidence: 99%

Air quality diagnosis from comprehensive observations of total OH reactivity and reactive trace species in urban central Tokyo

Yoshino

Nakashima

Miyazaki

et al. 2012

Atmospheric Environment

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a b s t r a c tWe have conducted a comprehensive observational study to determine the mixing ratios of atmospheric chemical species and total OH reactivity in central Tokyo, in order to diagnose the air quality during summer and winter 2007 and autumn 2009. Concentrations of over 70 reactive trace species were continuously measured throughout each season. The total OH reactivity was measured directly using a laser-induced pump and probe technique. The observed chemical species exhibited seasonal variations. There was a good correlation between NO and CO in winter, but not in summer. This indicates that during winter, vehicle exhaust provided a significant source of NO in central Tokyo, while photolysis of NO 2 was dominant in summer. Similar values (approximately 30 s À1 ) for the averaged total OH reactivity were observed in both summer and autumn during the daytime. However, VOCs accounted for a larger percentage of the OH reactivity in summer, while NO x was more dominant in autumn. We find that photochemical processes leading to oxidant production via VOCs dominated OH removal in summer, while the production of nitric acid from the reaction between OH and NO 2 was dominant in autumn, by-passing the oxidant production pathways and resulting in reduced oxidant formation.

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“…Recent literature points out that isoprene -the most important single VOC emitted from land vegetation -is poorly understood both in terms of gas phase oxidation mechanism (Lelieveld et al, 2008;Hofzumahaus et al, 2009;Paulot et al, 2009;Peeters and Müller, 2010) and its impact on new particle formation (Kiendler-Scharr et al, 2009b). Observations of atmospheric OH concentrations indicate that under low NO x conditions isoprene may be involved in a so far unidentified recycling mechanism that converts HO 2 into OH 1022 A. Kiendler-Scharr et al: Effects on new particle formation and OH concentrations without involving ozone formation (Tan et al, 2001;Thornton et al, 2002;Ren et al, 2008;Lelieveld et al, 2008;Hofzumahaus et al, 2009;Whalley et al, 2011;Lu et al, 2011).…”

Section: Introductionmentioning

confidence: 99%

“…Observations of atmospheric OH concentrations indicate that under low NO x conditions isoprene may be involved in a so far unidentified recycling mechanism that converts HO 2 into OH 1022 A. Kiendler-Scharr et al: Effects on new particle formation and OH concentrations without involving ozone formation (Tan et al, 2001;Thornton et al, 2002;Ren et al, 2008;Lelieveld et al, 2008;Hofzumahaus et al, 2009;Whalley et al, 2011;Lu et al, 2011). Contrary, suppression of new particle formation by isoprene was ascribed to its suppression of OH concentrations (Kiendler-Scharr et al, 2009b).…”

Section: Introductionmentioning

confidence: 99%

Isoprene in poplar emissions: effects on new particle formation and OH concentrations

Kiendler‐Scharr¹,

Andres²,

Bachner³

et al. 2012

Atmos. Chem. Phys.

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Abstract. Stress-induced volatile organic compound (VOC) emissions from transgenic Grey poplar modified in isoprene emission potential were used for the investigation of photochemical secondary organic aerosol (SOA) formation. In poplar, acute ozone stress induces the emission of a wide array of VOCs dominated by sesquiterpenes and aromatic VOCs. Constitutive light-dependent emission of isoprene ranged between 66 nmol m −2 s −1 in non-transgenic controls (wild type WT) and nearly zero (<0.5 nmol m −2 s −1 ) in isoprene emission-repressed plants (line RA22), respectively. Nucleation rates of up to 3600 cm −3 s −1 were observed in our experiments. In the presence of isoprene new particle formation was suppressed compared to non-isoprene containing VOC mixtures. Compared to isoprene/monoterpene systems emitted from other plants the suppression of nucleation by isoprene was less effective for the VOC mixture emitted from stressed poplar. This is explained by the observed high efficiency of new particle formation for emissions from stressed poplar. Direct measurements of OH in the reaction chamber revealed that the steady state concentration of OH is lower in the presence of isoprene than in the absence of isoprene, supporting the hypothesis that isoprenes' suppressing effect on nucleation is related to radical chemistry. In order to test whether isoprene contributes to SOA mass formation, fully deuterated isoprene (C 5 D 8 ) was added to the stress-induced emission profile of an isoprene free poplar mutant. Mass spectral analysis showed that, despite the isoprene-induced suppression of particle formation, fractions of deuterated isoprene were incorporated into the SOA. A fractional mass yield of 2.3 % of isoprene was observed. Future emission changes due to land use and climate change may therefore affect both gas phase oxidation capacity and new particle number formation.

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Amplified Trace Gas Removal in the Troposphere

Cited by 594 publications

References 25 publications

The impact of local surface changes in Borneo on atmospheric composition at wider spatial scales: coastal processes, land-use change and air quality

The impact of local surface changes in Borneo on atmospheric composition at wider spatial scales: coastal processes, land-use change and air quality

Air quality diagnosis from comprehensive observations of total OH reactivity and reactive trace species in urban central Tokyo

Isoprene in poplar emissions: effects on new particle formation and OH concentrations

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