Methyl bromide (CH₃Br) is a potent ozone-depleting substance (ODS) that has both natural and anthropogenic sources. CH₃Br has been used mainly for preplant soil fumigation, post-harvest grain and timber fumigation, and structural fumigation. Most non-quarantine and pre-shipment (non-QPS) uses were phased out by 2005 for non-Article 5 (developed) countries and by 2015 for Article 5 (developing) countries under the Montreal Protocol on Substances that Deplete the Ozone Layer; some uses have continued under critical-use exemptions (CUEs). Under the protocol, individual nations are required to report annual data on CH₃Br production and consumption for quarantine–pre-shipment (QPS) uses, non-QPS uses, and CUEs to the United Nations Environment Programme (UNEP). In this study, we analyzed high-precision, in situ measurements of atmospheric mole fractions of CH₃Br obtained at the Gosan station on Jeju Island, South Korea, from 2008 to 2019. The background mole fractions of CH₃Br in the atmosphere at Gosan declined from 8.5±0.8 ppt (parts per trillion) in 2008 to 7.4±0.6 ppt in 2019 at a rate of $-\mathrm{0.13}\pm \mathrm{0.02}$ ppt yr⁻¹. At Gosan, we also observed periods of persistent mole fractions (pollution events) elevated above the decreasing background in continental air masses from China. Statistical back-trajectory analyses showed that these pollution events are predominantly traced back to CH₃Br emissions from eastern China. Using an interspecies correlation (ISC) method with the reference trace species CFC-11 (CCl₃F), we estimate anthropogenic CH₃Br emissions from eastern China at an average of 4.1±1.3 Gg yr⁻¹ in 2008–2019, approximately 2.9±1.3 Gg yr⁻¹ higher than the bottom-up emission estimates reported to UNEP. Possible non-fumigation CH₃Br sources – rapeseed production and biomass burning – were assessed, and it was found that the discrepancy is most likely due to unreported or incorrectly reported QPS and non-QPS fumigation uses. These unreported anthropogenic emissions of CH₃Br are confined to eastern China and account for 30 %–40 % of anthropogenic global CH₃Br emissions. They are likely due to delays in the introduction of CH₃Br alternatives, such as sulfuryl fluoride (SO₂F₂), heat, and irradiation, and a possible lack of industry awareness of the need for regulation of CH₃Br production and use.

Hydrofluorocarbons (HFCs) are powerful anthropogenic greenhouse gases (GHGs) with high global-warming potentials (GWPs). They have been widely used as refrigerants, insulation foam-blowing agents, aerosol propellants, and fire suppression agents. Since the mid-1990s, emissions of HFCs have been increasing rapidly as they are used in many applications to replace ozone-depleting chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs) whose consumption and production have been phased out under the Montreal Protocol (MP). Due to the high GWP of HFCs, the Kigali Amendment to the MP requires the phasedown of production and consumption of HFCs to gradually achieve an 80 %–85 % reduction by 2047, starting in 2019 for non-Article 5 (developed) countries with a 10 % reduction against each defined baseline and later schedules for Article 5 (developing) countries. In this study, we have examined long-term high-precision measurements of atmospheric abundances of five major HFCs (HFC-134a, HFC-143a, HFC-32, HFC-125, and HFC-152a) at Gosan station, Jeju Island, South Korea, from 2008 to 2020. Background abundances of HFCs gradually increased, and the inflow of polluted air masses with elevated abundances from surrounding source regions were detected over the entire period. From these pollution events, we inferred regional and country-specific HFC emission estimates using two independent Lagrangian particle dispersion models and Bayesian inversion frameworks (FLEXPART-FLEXINVERT+ and NAME-InTEM). The spatial distribution of the derived “top-down” (measurement based) emissions for all HFCs shows large fluxes from megacities and industrial areas in the region. Our most important finding is that HFC emissions in eastern China and Japan have sharply increased from 2016 to 2018. The contribution of East Asian HFC emissions to the global total increased from 9 % (2008–2014) to 13 % (2016–2020). In particular, HFC emissions in Japan (Annex I country) rose rapidly from 2016 onward, with accumulated total inferred HFC emissions being ∼ 114 Gg yr⁻¹, which is ∼ 76 Gg yr⁻¹ higher for 2016–2020 than the “bottom-up” (i.e., based on activity data and emission factors) emissions of ∼ 38 Gg yr⁻¹ reported to the United Nations Framework Convention on Climate Change (UNFCCC). This is likely related to the increase in domestic demand in Japan for refrigerants and air-conditioning-system-related products and incomplete accounting. A downward trend of HFC emissions that started in 2019 reflects the effectiveness of the F-gas policy in Japan. Eastern China and South Korea, though not obligated to report to the UNFCCC, voluntarily reported emissions, which also show differences between top-down and bottom-up emission estimates, demonstrating the need for atmospheric measurements, comprehensive data analysis, and accurate reporting for precise emission management. Further, the proportional contribution of each country's CO₂-equivalent HFC emissions has changed over time, with HFC-134a decreasing and HFC-125 increasing. This demonstrates the transition in the predominant HFC substances contributing to global warming in each country.

Trifluoromethane (CHF₃, HFC-23), one of the most potent greenhouse gases among hydrofluorocarbons (HFCs), is mainly emitted to the atmosphere as a by-product in the production of the ozone-depleting legacy refrigerant and chemical feedstock chlorodifluoromethane (CHClF₂, HCFC-22). A recent study on atmospheric observation-based global HFC-23 emissions (top-down estimates) showed significant discrepancies over 2014–2017 between the increase in the observation-derived emissions and the 87 % emission reduction expected from capture and destruction processes of HFC-23 at HCFC-22 production facilities implemented by national phase-out plans (bottom-up emission estimates) (Stanley et al., 2020). However, the actual regions responsible for the increased emissions were not identified. Here, we estimate the regional top-down emissions of HFC-23 for eastern Asia based on in situ measurements at Gosan, South Korea, and show that the HFC-23 emissions from eastern China have increased from 5.0±0.4 Gg yr⁻¹ in 2008 to 9.5±1.0 Gg yr⁻¹ in 2019. The continuous rise since 2015 was contrary to the large emissions reduction reported under the Chinese hydrochlorofluorocarbons production phase-out management plan (HPPMP). The cumulative difference between top-down and bottom-up estimates for 2015–2019 in eastern China was $\sim \mathrm{23.7}\pm \mathrm{3.6}$ Gg, which accounts for 47±11 % of the global mismatch. Our analysis based on HCFC-22 production information suggests the HFC-23 emissions rise in eastern China is more likely associated with known HCFC-22 production facilities rather than the existence of unreported, unknown HCFC-22 production, and thus observed discrepancies between top-down and bottom-up emissions could be attributed to unsuccessful factory-level HFC-23 abatement and inaccurate quantification of emission reductions.

Clouds act as a major reflector that changes the amount of sunlight reflected to space. Change in radiance intensity due to the presence of clouds interrupts the retrieval of trace gas or aerosol properties from satellite data. In this paper, we developed a fast and robust algorithm, named the fast cloud retrieval algorithm, using a triplet of wavelengths (469, 477, and 485 nm) of the O₂–O₂ absorption band around 477 nm (CLDTO4) to derive the cloud information such as cloud top pressure (CTP) and cloud fraction (CF) for the Geostationary Environment Monitoring Spectrometer (GEMS). The novel algorithm is based on the fact that the difference in the optical path through which light passes with regard to the altitude of clouds causes a change in radiance due to the absorption of O₂–O₂ at the three selected wavelengths. To reduce the time required for algorithm calculations, the look-up table (LUT) method was applied. The LUT was pre-constructed for various conditions of geometry using Vectorized Linearized Discrete Ordinate Radiative Transfer (VLIDORT) to consider the polarization of the scattered light. The GEMS was launched in February 2020, but the observed data of GEMS have not yet been widely released. To evaluate the performance of the algorithm, the retrieved CTP and CF using observational data from the Global Ozone Monitoring Experiment-2 (GOME-2), which cover the spectral range of GEMS, were compared with the results of the Fast Retrieval Scheme for Clouds from the Oxygen A band (FRESCO) algorithm, which is based on the O₂ A-band. There was good agreement between the results, despite small discrepancies for low clouds.

The Geostationary Environment Monitoring Spectrometer (GEMS) is the first geostationary earth orbit (GEO) environmental instrument, onboard the Geostationary Korea Multi-Purpose Satellite–2B (GEO-KOMPSAT-2B) launched on 19 February 2020, and is measuring reflected radiance from the earth's surface and atmosphere system in the range of 300–500 nm in the ultraviolet–visible (UV–Vis) region. The radiometric response of a satellite sensor that measures the UV–Vis wavelength region can depend on the polarization states of the incoming light. To reduce the sensitivity due to polarization, many current low earth orbit (LEO) satellites are equipped with a scrambler to depolarize the signals or a polarization measurement device (PMD) that simultaneously measures the polarization state of the atmosphere, then utilizes it for a polarization correction. However, a novel polarization correction algorithm is required since GEMS does not have a scrambler or a PMD. Therefore, this study aims to improve the radiometric accuracy of GEMS by developing a polarization correction algorithm optimized for GEMS that simultaneously considers the atmosphere's polarization state and the instrument's polarization sensitivity characteristics. The polarization factor and axis were derived by the preflight test on the ground as a function of wavelengths, showing a polarization sensitivity of more than 2 % at some specific wavelengths. The polarization states of the atmosphere are configured as a look-up table (LUT) using the Vector Linearized Discrete Ordinate Radiative-Transfer model (VLIDORT). Depending on the observation geometry and atmospheric conditions, the observed radiance spectrum can include a polarization error of 2 %. The performance of the proposed GEMS polarization algorithm was assessed using synthetic data, and the errors due to polarization were found to be larger in clear regions than in cloudy regions. After the polarization correction, polarization errors were reduced close to zero for almost all wavelengths, including the wavelength regions with high peaks and curvatures in the GEMS polarization factor, which sufficiently demonstrates the effectiveness of the proposed polarization correction algorithm. From the actual observation data after the launch of GEMS, the diurnal variation for the spatial distribution of polarization error was confirmed to be minimum at noon and maximum at sunrise/sunset. This can be used to improve the quality of GEMS measurements, the first geostationary environmental satellite, and then contribute to the retrieved accuracy of various Level-2 products, such as trace gases and aerosols in the atmosphere.