Abstract

Abstract. To examine the influence of both crop cultivation and surface air temperatures (SATs) on annual global isoprene and monoterpene emissions, which can lead to the formation of secondary organic aerosols (SOAs), we simulated, on a monthly basis, the annual emissions of volatile organic compounds (VOCs) during the period 1854–2000. The model estimates were based on historical climate data such as SATs, and downward solar radiation (DSR) reproduced with an atmospheric-ocean circulation model, as well as a time series of the global distribution of cropland (to test the hypothesis that conversion of forests into croplands lowers emissions). The simulations demonstrated that global SAT, DSR, the combination of SAT and DSR, and the expansion of cropland all affected emissions. The effect of cropland expansion (i.e., forest conversion) on annual emissions during this period was larger for isoprene (~7% reduction on a global scale) than for monoterpenes (~2% reduction), mainly because of the reduction in broadleaf evergreen forests (BEFs) in Southeast Asia, which have the highest and most constant emissions of isoprene and where both temperature and radiation are high all year round. The reduction in the Amazon region and in parts of Africa, which are other primary sources of annual global isoprene emissions, but where the conversion of BEF to cropland has been much smaller than in Southeast Asia, was less remarkable, probably because the broadleaf deciduous forests and C4 grasslands in these areas have lower and seasonal emissions; hence, their conversion has less effect. On the other hand, the difference in the emission factors (ε) between cropland and the other vegetation types was much lower for monoterpenes than for isoprene, although the ε for cropland was generally the lowest for both compounds. Thus, the expansion of cropland also contributed to the reduction in monoterpene emissions to some degree, but had less effect. A ~5% increase in emissions due to rising SAT was more than offset by the decrease in isoprene emissions and a concurrent ~2% reduction caused by a decrease in DSR. Overall, annual global isoprene emissions in 2000 were lower than in 1854 by 13 TgC yr−1, whereas annual global monoterpene emissions were higher by 2.3 TgC yr−1.

Highlights

  • Monoterpene secondary organic aerosols (SOAs) are the most important organic aerosol components on a global scale (Chung and Seinfeld, 2002; Engelhart et al, 2008)

  • We estimated annual global isoprene and monoterpene emissions since the beginning of the industrial age (1850s) with the MEGAN model (Guenther et al, 2006), based on SAT and downward solar radiation (DSR) reconstructed by a historical run with MIROC5, and temporal expansion of cropland

  • We investigated the influences of SAT, DSR, and cropland expansion on both annual emissions

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Summary

Introduction

Monoterpene secondary organic aerosols (SOAs) are the most important organic aerosol components on a global scale (Chung and Seinfeld, 2002; Engelhart et al, 2008). Vegetation is thought to contribute to about 90 % of global emissions of volatile organic compounds (VOCs) (Kuhn et al, 2004), and Guenther et al (1995) estimated that the annual global VOC flux is 1150 TgC, composed of 44 % isoprene, 11 % monoterpenes, 22.5 % other reactive VOCs, and 22.5 % other VOCs. That study showed that the contribution to VOCs from vegetation should not be ignored when considering carbon cycles. The estimation of VOC emissions from vegetation, especially isoprene and monoterpene emissions, is essential for understanding global tropospheric chemistry and regional photochemical oxidant formation, for balancing the global carbon cycle, and for understanding the production of organic acids (Fehsenfeld et al, 1992)

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