Optimal design of surface CO2 observation network to constrain China's land carbon sink.

Accurate estimate of the size of land carbon sink is essential for guiding climate mitigation actions to fulfill China's net-zero ambitions before 2060. The atmospheric inversion is an effective approach to provide spatially explicit estimate of surface CO2 fluxes that are optimally consistent with atmospheric CO2 measurements. But atmospheric inversion of China's land carbon sink has enormous uncertainties, with one major source arising from the poor coverage of CO2 observation stations. Here we use a regional atmospheric inversion framework to design an observation network that could minimize uncertainties in inverted estimate of China's land carbon sink. Compared with the large spread of inverted sink (∼1PgCa-1) from state-of-the-art inversions using existing CO2 observations, the uncertainty is constrained within 0.3PgCa-1 when a total of 30 stations were deployed, and is further reduced to approximately 0.2PgCa-1 when 60 stations were deployed. The proposed stations are mostly distributed over areas with high biosphere productivity during the growing season, such as Southeast China, Northeast China, North China, and the Tibetan Plateau. Moreover, the proposed stations can cover areas where existing satellites have limited coverage due to cloud shadowing in the monsoon season or over complex topography. Such ground-based observation network will be a critical component in the future integrated observing system for monitoring China's land carbon fluxes.

Explosive formation of secondary organic aerosol due to aerosol-fog interactions.

Aerosol particles can profoundly affect the local environment and global climate. Explosive growths of secondary organic aerosol (SOA) are frequently observed during serious haze evens, but their fundamental mechanism remains unclear. We used chamber experiments and kinetic model simulations to reveal the microphysical mechanism for explosive organic aerosol formation. The evolution of SOA with organic vapors under dry and highly humid conditions was determined based on a high-resolution Orbitrap mass spectrometer. We found that the condensation of gas-phase organics could lead to the formation of cloud or fog droplets with relative humidity below 100 %; meanwhile, the aerosol-fog interaction could result in the explosive growth of SOA. Monomeric products from toluene oxidation were verified to primarily contribute to the increased SOA in super humid conditions, which are mainly assigned to be intermediate- and semi-volatile organic compounds. Moreover, we demonstrated that the decreasing temperatures could dramatically amplify organic compounds' co-condensing influence on SOA explosive formation and activation at relative humidity above 85 % and temperature below 20 °C. Our findings revealed that aerosol-fog interaction is the fundamental driving force for explosive organic aerosol formation. It indicates that overlooking the co-condensation of organic vapors with water could significantly underestimate SOA and liquid water content in 3D models.

Real-time characterization of aerosol particle composition, sources and influences of increased ventilation and humidity in an office.

Most of human exposure to atmospheric pollutants occurs indoors, and the components of outdoor aerosols may have been changed in the way before reaching indoor spaces. Here we conducted real-time online measurements of mass concentrations and chemical composition of black carbon and the non-refractory species in PM2.5 in an occupied office for approximately one month. The open-close windows and controlled dampness experiments were also performed. Our results show that indoor aerosol species primarily originate from outdoors with indoor/outdoor ratio of these species typically less than unity except for certain organic aerosol (OA) factors. All aerosol species went through filtration upon transport indoors. Ammonium nitrate and fossil fuel OA underwent evaporation or particle-to-gas partitioning, while less oxidized secondary OA (SOA) underwent secondary formation and cooking OA might have indoor sources. With higher particulate matter (PM) mass concentration outdoors than in the office, elevated natural ventilation increased PM exposure indoors and this increased exposure was prolonged when outdoor PM was scavenged. We found that increasing humidity in the office led to higher indoor PM mass concentration particularly more oxidized SOA. Overall, our results highlight that indoor exposure of occupants is substantially different from outdoor in terms of mass concentrations and chemical species.

Optical design of double-grating and double wave band spectrometers using a common CCD.

A new type of optical system comprising double-grating and double wave band spectrometers is designed for atmospheric detection. The optical system can bring oxygen A band (758-778 nm) and water vapor absorption band (758-880 nm) on a charge-coupled device (CCD) at the same time for ultrahigh resolution spectrum measurement. Each absorbed band with three observation directions of atmospheric radiation is imaged in different positions of a common CCD. The spectral resolution is less than 0.07 nm in oxygen A band (758-778 nm), and the spectral resolution is less than 0.28 nm in water vapor absorption band (758-880 nm). Three end faces of the optical fiber are on the slit plane for each wave band, and each end face corresponds to an observation angle. The optical fiber core diameter is 600 µm, the slit width is 25 µm, and the slit length is 18.4 mm. The principle of smile correction is analyzed. The smile of the Czerny-Turner double-grating spectrometer can be compensated by using the tilt field lens in front of the focal plane. The design results corroborate that the maximum smile of the double-grating spectrometer is 5 µm and that the approach of correcting smile is effective. The stray light is analyzed, and the approaches of suppressing the stray light are proposed.

[Factors Analysis for CO2 Retrieval from the Ground-Based Hyperspectral Measurements in the Short Wave Infrared].

Ground-based CO2 inversion accuracy determines the understanding of CO2 source and sink. However the study about factors affecting ground-based CO2 inversion. In order to improve CO2 inversion accuracy, the effects from aerosol, spectral shift, spectral band selection, spectrometer response function type, half width and truncation error have been analyzed by using radiative transfer model. The results show that: (1) the multiple scattering of aerosol can be ignored when instrument field of view is less than 1.5° and aerosol optical depth is less than 0.5. (2) The inversion results are smaller when there are spectral offsets. The inversion errors increase nonlinear with spectral offsets. And the higher the spectral resolution, the larger the effect of spectral shift. (3) Different spectral bands have various average signal-to-noise ratio, selecting channels with appropriate signal-to-noise ratio and enhancing instrument signal-to-noise ratio can reduce the effect of instrument noise. (4) The higher the instrument resolution, the more important the degree of accuracy of instrument line function for simulated spectrum. Therefore, for hyper-spectral observation, the constancy of environmental temperature is key of acquiring high precision inversion results. (5) For over-high spectral resolution, simulated spectrum is anamorphic due to crosstalk effect. Therefore the crosstalk effect must be considered when the spectrometer resolution is advanced.

Impact of vertical stratification of inherent optical properties on radiative transfer in a plane-parallel turbid medium.

The atmosphere is often divided into several homogeneous layers in simulations of radiative transfer in plane-parallel media. This artificial stratification introduces discontinuities in the vertical distribution of the inherent optical properties at boundaries between layers, which result in discontinuous radiances and irradiances at layer interfaces, which lead to errors in the radiative transfer simulations. To investigate the effect of the vertical discontinuity of the atmosphere on radiative transfer simulations, a simple two layer model with only aerosols and molecules and no gas absorption is used. The results show that errors larger than 10% for radiances and several percent for irradiances could be introduced if the atmosphere is not layered properly.