The light absorption enhancement (E-abs) of black carbon (BC) coated with non-BC materials is crucial in the assessment of radiative forcing, yet its evolution during photochemical aging of plumes from biomass burning, the globe's largest source of BC, remains poorly understood. In this study, plumes from open burning of corn straw were introduced into a smog chamber to explore the evolution of E-abs during photochemical aging. The light absorption of BC was measured with and without coating materials by using a thermodenuder, while the size distributions of aerosols and composition of BC coating materials were also monitored. E-abs was found to increase initially, and then decrease with an overall downward trend. The lensing effect dominated in E-abs at 520 nm, with an estimated contribution percentages of 47.5%-94.5%, which is far greater than light absorption of coated brown carbon (BrC). The effects of thickening and chemical composition changes of the coating materials on E-abs were evaluated through comparing measured E-abs with that calculated by the Mie theory. After OH exposure of 1 x 10(10) molecules cm(-3) s, the thickening of coating materials led to an E-abs increase by 3.2% +/- 1.6%, while the chemical composition changes or photobleaching induced an E-abs decrease by 4.7% +/- 0.6%. Simple forcing estimates indicate that coated BC aerosols exhibit warming effects that were reduced after aging. The oxidation of light-absorbing CxHy compounds, such as polycyclic aromatic hydrocarbons (PAHs), to CxHyO and CxHyO>1 compounds in coating materials may be responsible for the photobleaching of coated BrC. Plain Language Summary Understanding how black carbon (BC) coated with non-BC materials affects light absorption is crucial for assessing its impact on the Earth's climate. However, there is limited knowledge about how this process changes when BC, particularly from biomass burning, is exposed to light. Biomass burning is a significant global source of BC. This study investigated the changes in light absorption of BC from burning corn straw as it aged in a controlled environment. We measured the light absorption of BC with and without its coating materials. Our results showed that the main cause of increased light absorption was the lensing effect of the coating materials, which was more significant than the light absorption by the coating materials themselves. We also discovered that as the coating materials thickened, BC absorbed more light. However, changes in the chemical composition of the coating materials led to a decrease in total absorption. These findings suggest that while coated BC initially has a warming effect on the climate, this effect diminished as the BC ages. The decrease is likely due to the breakdown of light-absorbing compounds in the coating materials, such as polycyclic aromatic hydrocarbons (PAHs).

High uncertainty in optical properties of black carbon (BC) involving heterogeneous chemistry has recently attracted increasing attention in the field of atmospheric climatology. To fill the gap in BC optical knowledge so as to estimate more accurate climate effects and serve the response to global warming, it is beneficial to conduct site-level studies on BC light absorption enhancement (E-abs) characteristics. Real-time surface gas and particulate pollutant observations during the summer and winter over Wuhan were utilized for the analysis of E-abs simulated by minimum R squared (MRS), considering two distinct atmospheric conditions (2015 and 2017). In general, differences in aerosol emissions led to E-abs differential behaviors. The summer average of E-abs (1.92 +/- 0.55) in 2015 was higher than the winter average (1.27 +/- 0.42), while the average (1.11 +/- 0.20) in 2017 summer was lower than that (1.67 +/- 0.69) in winter. E-abs and R-BC (representing the mass ratio of non-refractory constituents to elemental carbon) constraints suggest that E-abs increased with the increase in R-BC under the ambient condition enriched by secondary inorganic aerosol (SIA), with a maximum growth rate of 70.6% in 2015 summer. However, E-abs demonstrated a negative trend against R-BC in 2017 winter due to the more complicated mixing state. The result arose from the opposite impact of hygroscopic SIA and absorbing OC/irregular distributed coatings on amplifying the light absorbency of BC. Furthermore, sensitivity analysis revealed a robust positive correlation (R > 0.9) between aerosol chemical compositions (including sulfate, nitrate, ammonium and secondary organic carbon), which could be significantly perturbed by only a small fraction of absorbing materials or restructuring BC through gaps filling. The above findings not only deepen the understanding of BC, but also provide useful information for the scientific decision-making in government to mitigate particulate pollution and obtain more precise BC radiative forcing.

Black carbon (BC) is a distinct type of carbonaceous aerosol that has a significant impact on the environment, human health, and climate. A non-BC material coating on BC can alter the mixing state of the BC particles, which considerably enhances the mass absorption efficiency of BC by directing more energy toward the BC cores (lensing effect). A lot of methods have been reported for quantifying the enhancement factor (Eabs), with diverse results. However, to the best of our knowledge, a comprehensive review specific to the quantification methods for Eabs has not been systematically performed, which is unfavorable for the evaluation of obtained results and subsequent radiative forcing. In this review, quantification methods are divided into two broad categories, direct and indirect, depending on whether experimental removal of the coating layer from an aged carbonaceous particle is required. The direct methods described include thermal peeling, solvent dissolution, and optical virtual exfoliation, while the indirect methods include intercept-linear regression fitting, minimum R squared, numerical simulation, and empirical value. We summarized the principles, procedures, virtues, and limitations of the major Eabs quantification methods and analyzed the current problems in the determination of Eabs. We pointed out what breakthroughs are needed to improve or innovate Eabs quantification methods, particularly regarding the need to avoid the influence of brown carbon, develop a broadband Eabs quantification scheme, quantify the Eabs values for the emissions of low-efficiency combustions, measure the Eabs of particles in a highhumidity environment, design a real-time monitor of Eabs by a proper combination of mature techniques, and make more use of artificial intelligence for better Eabs quantification. This review deepens the understanding of Eabs quantification methods and benefits the estimation of the contribution of BC to radiative forcing using climate models.

By quantifying the absorption of black carbon (BC), brown carbon (BrC) and the lensing effect, we found that BrC dominates the total absorption at 450 nm, and the largest absorption contribution proportion of BrC could reach 78.3% during heavy pollution. The average absorption enhancement (E-abs) at 530 nm was only 1.38, indicating that BC is not coated well here. The average value of the absorption Angstrom exponent (AAE) between 450 nm and 530 nm was 5.3, suggesting a high concentration of BrC in Wangdu. CHN+ was the greatest contributor to the light absorption of molecules detected in MSOC with a proportion of 12.2-22.4%, in which the polycyclic aromatic nitrogen heterocycles (PANHs) were the dominant compounds. The C6H5NO3 and its homologous series accounted for 3.0-11.3%, and the C15H9N and its homologous series, including one C16H11N and three C17H13N compounds, accounted for 5.1-12.3%. The absorption of these PANHs is comparable to that of nitro-aromatics, which should attract more attention to the impact of climate radiative forcing.

Black carbon (BC) is one important component contributing to global warming and its climate-related impacts strongly depend on mixing state. Previous observations at ground level indicated BC aging was at a fast rate in daytime with efficient photochemical reactions, while BC aging significantly weakened at night. Here we present evidences that BC aging still occurs efficiently at night in the residual layer (RL). The ratio of thickly coated refractory BC (rBC) in total rBC (f(BC)) increased from 51.3% at 00:00 LST to 61.5% at 07:00 LST at the CITIC station, which located in the RL at night, with an increasing rate of 1.4% per hour. Such an increasing rate was even higher than that during noontime (11:00 to 15:00 LST, 0.7% per hour). Similar trend also reflected in the coating thickness (Dp/Dc) of rBC particles, which increased from 1.52 at 00:00 LST to 1.63 at 07:00 LST. The aging of rBC in the RL at night enhances light absorption of rBC particles correspondingly; calculated absorption enhancement (E-abs) increased from 1.64 at 00:00 LST to 1.79 in at 07:00 LST. Further analysis indicated that the Eabs depends not only on the D-p/D-c of rBC particles, but also on its size. An increase in the size of rBC particles in polluted episode can also enhance the Eabs. Combined observations of development of boundary layer and pollutants at the CITIC station suggested that rBC particles were upwards transported in daytime and trapped in the RL at night, where they were aged efficiently. These results will improve our understanding on rBC aging in the atmosphere, and hence help to evaluate its radiative forcing.

The addition of coating to the black carbon (BC) enhances its absorption as more light is focused by the coating lens. The absorption enhancement factor (E-abs) of BC is difficult to quantify due to an inadequate representation of its mixing structure and the interaction with radiation. Here, by tracking the evolution of the fresh BC particles in the ambient, we found a transitional stage of the particle E-abs with the non-BC-to-BC mass ratio (R-BC) at similar to 2, below which there were insufficient coating materials to encapsulate the BC core and the absorption enhancement was not significant (similar to 14%). When the R-BC >similar to 2, obvious absorption enhancement occurred as the BC cores were fully covered. Secondary inorganic species played the most critical role in the coating materials to enhance the lensing effect. We suppose the particle-resolved core-shell Mie model can be applied in the E-abs prediction for most cases.

The radiative forcing of soot is dependent on the morphology, mixing state and structure. Cloud processing has been predicted to affect their mixing properties but little is known about the resulting light absorption properties. We collected ambient particles in the pre-cloud period, the cloud residues and interstitials in the in-cloud period at Mt. Tianjing (southern China). The morphology parameters of soot aggregates with varying mixing materials [sulfate (S) and organics (OM)] and mixing structures were investigated by a transmission electron microscope, and their absorption cross were calculated based on discrete dipole approximation. We found that the number contribution of soot-S decreased from 45% in the pre-cloud period to 32% in the in-cloud period, and that of soot-OM increased from 44% to 60%. Moreover, the number proportion of soot-OM with fully embedded structure increased remarkably in the in-cloud period (29%), compared with that in the pre-cloud period (3%). In addition, the soot-S aggregates became denser after in-cloud aqueous process. However, for soot-OM aggregates, the morphology remained relatively constant. The distinctly different change of soot-S and soot-OM in morphology highlights the chemically resolved reconstruction of soot morphology. Theoretical calculation further shows that the changes of soot particles in the mixing state and morphological characteristics by the cloud process resulted in the light absorption enhancement increase from 1.57 to 2.01. This study highlights that the evolution of microphysical properties upon cloud processing should also be considered in climate models to more accurately evaluate the impacts of soot particles.

Black carbon (BC) is estimated to have the second largest anthropogenic radiative forcing in earth-systems models (ESMs), but there is significant uncertainty in its impact due to complex mixing with organics. Laboratory-generated particles show that co-mixed non-absorbing material enhances absorption by BC by a factor of 2-3.5 as predicted by optical models. However, weak or no enhancements are often reported for field studies. The cause of lower-than-expected absorption is not well understood and implies a lower radiative impact of BC compared to how many ESMs currently treat aerosols. By analyzing BC aerosol particle-by-particle we reconcile observed and expected absorption for ambient smoke plumes varying in geographic origin, fuel types, burn conditions, atmospheric age and transport. Although particle-by-particle tracking is computationally prohibitive for sophisticated ESMs we show that realistic BC absorption is reliably estimated by bulk properties of the plume providing a suitable parameterization to constrain black carbon radiative forcing.

The significant uncertainty associated with black carbon (BC) radiative forcing estimation is mainly due to discrepancies related to its mixing state. The in situ measurement-based understanding of absorption properties is limited to only a few locations worldwide, primarily as a result of the unavailability of sophisticated instrumentations for absorption enhancement (Eabs) measurements resulting from mixing with non-BC chemicals. Therefore, we have proposed an alternative approach for a more robust in situ measurement of absorption enhancement using a thermal-optical carbon analyzer. In the present study, the absorption spectra during different stages of thermal-optical carbon analysis were used to estimate the absorption coefficients of mixed and pure BC aerosols. Moreover, we have also explored the possibility of apportioning light absorption by the BC core and absorbing organics (brown carbon). The present method was applied on a few ground-based aerosol samples collected at two distinct Indo-Gangetic Plain (IGP) sampling stations. Eabs at 808 nm was observed to be approximately 1.2 at both of the sampling sites. Interestingly, the absorbing brown carbon chromophores showed a wide range of absorption in the ultraviolet to near-infrared wavelengths with minimum absorption at 635 nm. Thus, the present study suggests that the absorption of organics in near-infrared wavelengths cannot be neglected.

Atmospheric black carbon (BC) has a large yet highly uncertain contribution to global warming. When mixed with non-BC/coating material during atmospheric aging, the BC light absorption can be enhanced through the lensing effect. Laboratory and modeling studies have consistently found strong BC absorption enhancement, while the results in ambient measurements are conflicting, with some reporting weak absorption enhancement even for particles with large bulk coating amounts. Here, from our direct field observations, we report both large and minor absorption enhancement factors for different BC-containing particle populations with large bulk non-BC-to-BC mass ratios. By gaining insights into the measured coating material distribution across each particle population, we find that the level of absorption enhancement is strongly dependent on the particle-resolved mixing state. Our study shows that the greater mixing-state heterogeneity results in the larger difference between observed and predicted absorption enhancement. We demonstrate that by considering the variability in coating material thickness in the optical model, the previously observed model measurement discrepancy of absorption enhancement can be reconciled. The observations and improved optical models reported here highlight the importance of mixing-state heterogeneity on BC's radiative forcing, which should be better resolved in large-scale models to increase confidence when estimating the aerosol radiation effect.