Arctic tropospheric ozone: assessment of current knowledge and model performance

Arctic tropospheric ozone: assessment of current knowledge and model performance
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DOI:
10.5194/acp-23-637-2023
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发表时间:
2023-01
影响因子:
6.3
通讯作者:
C. Whaley;K. Law;J. Hjorth;H. Skov;R. Stephen;Arnold;J. Langner;J. Pernov;R. Chien;J. Christensen;M. Deushi;Xinyi Dong;G. Faluvegi;M. Flanner;J. Fu;Michael;Gauss;U. Im;L. Marelle;T. Onishi;N. Oshima;D. Plummer;L. Pozzoli;Jean-Christophe Raut;R. Skeie;M. Thomas;Kostas;Tsigaridis;S. Tsyro;S. Turnock;K. Salzen;D. Tarasick
C. Whaley;K. Law;J. Hjorth;H. Skov;R. Stephen;Arnold;J. Langner;J. Pernov;R. Chien;J. Christensen;M. Deushi;Xinyi Dong;G. Faluvegi;M. Flanner;J. Fu;Michael;Gauss;U. Im;L. Marelle;T. Onishi;N. Oshima;D. Plummer;L. Pozzoli;Jean-Christophe Raut;R. Skeie;M. Thomas;Kostas;Tsigaridis;S. Tsyro;S. Turnock;K. Salzen;D. Tarasick
中科院分区:
地球科学1区
文献类型:
--
作者:
C. Whaley;K. Law;J. Hjorth;H. Skov;R. Stephen;Arnold;J. Langner;J. Pernov;R. Chien;J. Christensen;M. Deushi;Xinyi Dong;G. Faluvegi;M. Flanner;J. Fu;Michael;Gauss;U. Im;L. Marelle;T. Onishi;N. Oshima;D. Plummer;L. Pozzoli;Jean-Christophe Raut;R. Skeie;M. Thomas;Kostas;Tsigaridis;S. Tsyro;S. Turnock;K. Salzen;D. Tarasick

文献摘要

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抽象的。对流层臭氧(O3)是继二氧化碳(CO2)和甲烷(CH 4)之后的第三大温室气体(GHG),也是一种对人类健康和生态系统造成危害的大气污染物。这项研究汇集了最近对北极对流层O3观测和建模的研究,北极是一个迅速变暖和敏感的环境。在北极的不同地点,观测到的地表O3季节性循环有很大的不同。例如,北极沿海地区在春季由于表面溴化学造成的O3消耗事件而达到最低值。相比之下,其他北极地区在春季达到最大值。本研究中使用的12个最先进的模型缺乏模拟春季北极沿海表面O3消耗所需的表面卤素化学;然而,多模型中值(MMM)在北极非沿海地区具有准确的季节性周期。有大量的模型之间的变化,这是以前报道过的,我们表明,仍然没有收敛模型之间或模拟对流层O3及其前体物种的精度提高。MMM低估了北极表面O3的5%至15%,具体取决于位置。本文利用臭氧探空仪的观测资料和模式资料研究了对流层O_3的垂直分布。这些模型具有高度可变性,根据模型和高度,在± 50%的范围内模拟自由对流层O3。MMM的表现最好,在大多数地点和季节都在± 8%以内。然而,几乎所有的模式都高估了对流层顶附近的O3(10300 hPa或10800 km),这可能是由于低估对流层顶的高度和平流层O3在高纬度地区过度向下传输的持续问题。例如,MMM在尤里卡偏高约20%。观测和模拟的O3前体(CO,NOx和水库PAN)在整个对流层进行评估。模型低估了冬季CO无处不在,可能是由于低估CO排放量和可能高估OH的组合。在整个垂直剖面中(与飞机测量值相比),MMM低估了CO和NOx,但高估了PAN。也许是由于竞争的不足,MMM O3与观测到的O3相当好地匹配。我们的研究结果表明,尽管在过去的十年中模型更新,模型结果是高度可变的,并没有增加代表北极对流层O3的准确性。
Abstract. As the third most important greenhouse gas (GHG) after carbon dioxide (CO2) and methane (CH4), tropospheric ozone (O3) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O3 depletion events resulting from surface bromine chemistry. In contrast, other Arctic locations have a maximum in the spring. The 12 state-of-the-art models used in this study lack the surface halogen chemistry needed to simulate coastal Arctic surface O3 depletion in the springtime; however, the multi-model median (MMM) has accurate seasonal cycles at non-coastal Arctic locations. There is a large amount of variability among models, which has been previously reported, and we show that there continues to be no convergence among models or improved accuracy in simulating tropospheric O3 and its precursor species. The MMM underestimates Arctic surface O3 by 5 % to 15 % depending on the location. The vertical distribution of tropospheric O3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O3 within a range of ±50 % depending on the model and the altitude. The MMM performs best, within ±8 % for most locations and seasons. However, nearly all models overestimate O3 near the tropopause (∼300 hPa or ∼8 km), likely due to ongoing issues with underestimating the altitude of the tropopause and excessive downward transport of stratospheric O3 at high latitudes. For example, the MMM is biased high by about 20 % at Eureka. Observed and simulated O3 precursors (CO, NOx, and reservoir PAN) are evaluated throughout the troposphere. Models underestimate wintertime CO everywhere, likely due to a combination of underestimating CO emissions and possibly overestimating OH. Throughout the vertical profile (compared to aircraft measurements), the MMM underestimates both CO and NOx but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O3 matches the observed O3 reasonably well. Our findings suggest that despite model updates over the last decade, model results are as highly variable as ever and have not increased in accuracy for representing Arctic tropospheric O3.