北极平流层臭氧低值事件中的反硝化过程

Denitrification Process of Low-ozone Events in the Arctic Stratosphere

  • 摘要: 基于三维大气化学传输模式SLIMCAT模拟与微波临边探测仪(microwave limb sounder, MLS)的观测数据, 对比分析2010年12月—2011年3月和2019年12月—2020年3月北极平流层的反硝化过程。结果表明:考虑微物理过程的拉格朗日粒子沉降反硝化方案(denitrification by Lagrangian particle sedimentation, DLAPSE)的SLIMCAT能够更准确模拟北极平流层的反硝化过程。在456 K等熵面上, 热力学平衡方案模拟的北极地区HNO3的体积混合比较DLAPSE方案的结果偏低约11%, 前者高估了平流层低层的反硝化程度。随着北极冬季平流层温度降低, 热力学平衡方案模拟的HNO3体积混合比先升高后降低, 发生转变的临界温度高于DLAPSE方案, 导致硝酸三水合物粒子在相对较高的温度开始沉降, 这是热力学平衡方案高估平流层低层反硝化过程的可能原因。与2010年12月—2011年3月相比, 2019年12月—2020年3月北极平流层极涡强度更强, 且持续低温特征更显著, 这促使硝酸三水合物粒子更早形成并发生沉降, 导致后者的反硝化过程更强。

     

    Abstract: The denitrification process involves the removal of reactive nitrogen from stratospheric air masses through the gravitational sedimentation of nitric acid trihydrate particles in polar stratospheric clouds. This process delays the deactivation of reactive chlorine, thereby prolonging the duration of spring ozone depletion and intensifying its magnitude. Using the three-dimensional atmospheric chemical transport model SLIMCAT with different denitrification schemes, numerical simulation study is conducted on two distinct Arctic stratospheric ozone depletion events occurring from December 2010 to March 2011 and from December 2019 to March 2020. Through comparison of the simulation data with observations from the microwave limb sounder (MLS), the denitrification processes during these two events are thoroughly analyzed, and the model's capability to simulate stratospheric chemical composition and denitrification under different schemes is comprehensively evaluated. Results show that, compared to the thermodynamic equilibrium scheme, SLIMCAT model incorporating the Denitrification by Lagrangian Particle Sedimentation (DLAPSE) scheme, which considers microphysical processes, yields a more accurate representation of denitrification in the lower Arctic stratosphere. During both ozone depletion events, the simulated volume mixing ratio of HNO3 on 456 K isentropic surface in the Arctic region is lower under the thermodynamic equilibrium scheme than under DLAPSE scheme, with an average relative difference of approximately -11%. Consistently, the simulated ClO volume mixing ratio in March is about 10% higher, while O3 volume mixing ratio is about 4% lower. These results indicate that the thermodynamic equilibrium scheme overestimates the denitrification process in the lower stratosphere, which in turn delays the deactivation of ClOx. It leads to an overestimation of ClOx volume mixing ratio and consequently an overestimation of O3 depletion in the Arctic stratosphere. As the temperature in the Arctic winter stratosphere decreases, HNO3 volume mixing ratio simulated by the thermodynamic equilibrium scheme initially increases and then decreases, with the transition occurring at a higher critical temperature than in DLAPSE scheme. This leads to the sedimentation of nitric acid trihydrate particles starting at relatively higher temperatures during the cooling process, resulting in greater removal of HNO3. This phenomenon may explain the overestimation of denitrification in the lower Arctic stratosphere by the thermodynamic equilibrium scheme. Compared to the period from December 2010 to March 2011, the Arctic stratospheric polar vortex from December 2019 to March 2020 exhibits greater stability and intensity, along with more persistent low temperatures. These favorable conditions facilitate the earlier formation and sustained sedimentation of larger nitric acid trihydrate particles in the polar stratosphere, leading to enhanced HNO3 removal and consequently stronger denitrification in the lower stratosphere during the latter period. The findings of this study contribute significantly to improving the simulation of polar stratospheric clouds and ozone in chemical transport models.

     

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