Indirect Forcing Research Articles

Improving Aerosol Radiative Forcing and Climate in E3SM: Impacts of New Cloud Microphysics and Improved Wet Removal Treatments

AbstractNumerous Earth system models exhibit excessive aerosol effective forcing at the top of the atmosphere (TOA), including the Department of Energy's Energy Exascale Earth System Model (E3SM). Here, in the context of the E3SM version 3 effort, the predicted particle property (P3) stratiform cloud microphysics scheme and an enhanced deep convection parameterization suite (ZM_plus) are implemented into E3SM. The ZM_plus includes a convective cloud microphysics scheme, a multi‐scale coherent structure parameterization for mesoscale convective systems, and a revised cloud base mass flux formulation considering impacts of the large‐scale environment. The P3 scheme improved cloud and radiation particularly over the Northern Hemisphere and the frequency of heavy precipitation over the tropics, and the ZM_plus improved clouds in the tropics. P3 decreases aerosol effective forcing by 0.15 W m−2, while the ZM_plus increases it by 0.27 W m−2, resulting from excessive direct (0.31 W m−2) and indirect forcing (−1.79 W m−2). The excessive aerosol forcings are due to aerosol overestimation associated with insufficient aerosol wet removal. By improving the physical treatments in the aerosol wet removal, we effectively mitigate anthropogenic aerosol overestimation and thus attenuate direct (0.09 W m−2) and indirect aerosol forcing (−1.52 W m−2). Adjustment to primary organic matter hygroscopicity reduces direct and indirect forcing to more reasonable values: −0.13 W m−2 and −1.31 W m−2, respectively. On climatology, improved aerosol treatments mitigate overestimation of aerosol optical depth.

Sensitivity of cloud microphysics to aerosol is highly associated with cloud water content: Implications for indirect radiative forcing

The sensitivity of cloud microphysics to aerosol loading, quantified by the aerosol-cloud interactions (ACI) index, plays a crucial role in calculating the radiative forcing due to ACI (RFaci). However, the dependence of the ACI index on liquid water content (LWC) and its impact on RFaci are often overlooked. This study aims to investigate this dependence and evaluate its implications for RFaci, based on ground in-situ aerosol-cloud observations on Mt. Lu in eastern China. The results demonstrate that the ACI index exhibits an initial increase, followed by a decline with increasing LWC. In the unconstrained LWC scenario, the ACI index, calculated based on cloud droplet number concentration (ACIn of 0.13), is found to be lower than the lower bound of ACIn (0.17 to 0.35) obtained from the constrained LWC scenario. Neglecting this LWC-dependence leads to a significant underestimation of the mean RFaci by 53%. Furthermore, when calculating RFaci using the ACI index from droplet effective diameter (ACId), implying the neglect of the dispersion effect by assuming a fixed droplet spectrum width, it results in an overestimation of RFaci by 22% compared to using ACIn. These findings shed new light on the assessment of RFaci and help reconcile differences between observed and simulated RFaci. Plain language summaryAerosol-cloud interactions are the major source of uncertainty in understanding human-induced climate change. This study focused on the relationship between aerosol and clouds, specifically investigating how the sensitivity of cloud properties to aerosol loading associates with the amount of liquid water present in the clouds. Using ground in-situ observations of clouds and aerosols on Mt. Lu in eastern China, this study showed that the sensitivity of cloud properties to aerosol loading initially increases and then decreases as the cloud water content increases. Neglecting this dependence can lead to a significant underestimation of the impact of aerosol-cloud interactions on climate. These findings provide valuable insights for improving our understanding of how aerosols and clouds interact and contribute to climate change.

Use of an uncrewed aerial system to investigate aerosol direct and indirect radiative forcing effects in the marine atmosphere

Abstract. An uncrewed aerial system (UAS) has been developed for observations of aerosol and cloud properties relevant to aerosol direct and indirect forcing in the marine atmosphere. The UAS is a Hybrid Quadrotor–fixed-wing aircraft designed for launch and recovery from a confined space such as a ship deck. Two payloads, clear sky and cloudy sky, house instrumentation required to characterize aerosol radiative forcing effects. The observing platform (UAS plus payloads) has been deployed from a ship and from a coastal site for observations in the marine atmosphere. We describe here details of the UAS, the payloads, and first observations from the TowBoatU.S. Richard L. Becker (March 2022) and from the Tillamook UAS Test Range (August 2022). The development of this UAS technology for flights from ships and coastal locations is expected to greatly increase observations of aerosol radiative effects in the marine boundary layer over both temporal and spatial scales.

Larger Cloud Liquid Water Enhances Both Aerosol Indirect Forcing and Cloud Radiative Feedback in Two Earth System Models

AbstractPrevious studies have noticed that the Coupled Model Intercomparison Project Phase 6 (CMIP6) models with a stronger cooling from aerosol‐cloud interactions (ACI) also have an enhanced warming from positive cloud feedback, and these two opposing effects are counter‐balanced in simulations of the historical period. However, reasons for this anti‐correlation are less explored. In this study, we perturb the cloud ice microphysical processes to obtain cloud liquid of varying amounts in two Earth System Models (ESMs). We find that the model simulations with a larger liquid water path (LWP) tend to have a stronger cooling from ACI and a stronger positive cloud feedback. More liquid clouds in the mean‐state present more opportunities for anthropogenic aerosol perturbations and also weaken the negative cloud feedback at middle to high latitudes. This work, from a cloud state perspective, emphasizes the influence of the mean‐state LWP on effective radiative forcing due to ACI (ERFACI).

Observational evidence of strong forcing from aerosol effect on low cloud coverage.

Aerosols cool Earth's climate indirectly by increasing low cloud brightness and their coverage (Cf), constituting the aerosol indirect forcing (AIF). The forcing partially offsets the greenhouse warming and positively correlates with the climate sensitivity. However, it remains highly uncertain. Here, we show direct observational evidence for strong forcing from Cf adjustment to increased aerosols and weak forcing from cloud liquid water path adjustment. We estimate that the Cf adjustment drives between 52% and 300% of additional forcing to the Twomey effect over the ocean and a total AIF of -1.1 ± 0.8 W m-2. The Cf adjustment follows a power law as a function of background cloud droplet number concentration, Nd. It thus depends on time and location and is stronger when Nd is low. Cf only increases substantially when background clouds start to drizzle, suggesting a role for aerosol-precipitation interactions. Our findings highlight the Cf adjustment as the key process for reducing the uncertainty of AIF and thus future climate projections.

Generalized Aerosol/Chemistry Interface (GIANT): A Community Effort to Advance Collaborative Science across Weather and Climate Models

Abstract Atmospheric aerosol and chemistry modules are key elements in Earth system models (ESMs), as they predict air pollutant concentrations and properties that can impact human health, weather, and climate. The current uncertainty in climate projections is partly due to the inaccurate representation of aerosol direct and indirect forcing. Aerosol/chemistry parameterizations used within ESMs and other atmospheric models span large structural and parameter uncertainties that are difficult to assess independently of their host models. Moreover, there is a strong need for a standardized interface between aerosol/chemistry modules and the host model to facilitate portability of aerosol/chemistry parameterizations from one model to another, allowing not only a comparison between different parameterizations within the same modeling framework, but also quantifying the impact of different model frameworks on aerosol/chemistry predictions. To address this need, we have initiated a new community effort to coordinate the construction of a Generalized Aerosol/Chemistry Interface (GIANT) for use across weather and climate models. We aim to organize a series of community workshops and hackathons to design and build GIANT, which will serve as the interface between a range of aerosol/chemistry modules and the physics and dynamics components of atmospheric host models. GIANT will leverage ongoing efforts at the U.S. modeling centers focused on building next-generation ESMs and the international AeroCom initiative to implement this common aerosol/chemistry interface. GIANT will create transformative opportunities for scientists and students to conduct innovative research to better characterize structural and parametric uncertainties in aerosol/chemistry modules, and to develop a common set of aerosol/chemistry parameterizations.

Comparison of methods to estimate aerosol effective radiative forcings in climate models

Abstract. Uncertainty in the effective radiative forcing (ERF) of climate primarily arises from the unknown contribution of aerosols, which impact radiative fluxes directly and through modifying cloud properties. Climate model simulations with fixed sea surface temperatures but perturbed atmospheric aerosol loadings allow for an estimate of how strongly the planet's radiative energy budget has been perturbed by the increase in aerosols since pre-industrial times. The approximate partial radiative perturbation (APRP) technique further decomposes the contributions to the direct forcing due to aerosol scattering and absorption and to the indirect forcing due to aerosol-induced changes in cloud scattering, amount, and absorption, as well as the effects of aerosols on surface albedo. Here we evaluate previously published APRP-derived estimates of aerosol effective radiative forcings from these simulations conducted in the sixth phase of the Coupled Model Intercomparison Project (CMIP6) and find that they are biased as a result of two large coding errors that – in most cases – fortuitously compensate. The most notable exception is the direct radiative forcing from absorbing aerosols, which is more than 40 % larger averaged across CMIP6 models in the present study. Correcting these biases eliminates the residuals and leads to better agreement with benchmark estimates derived from double calls to the radiation code. The APRP method – when properly implemented – remains a highly accurate and efficient technique for diagnosing aerosol ERF in cases where double radiation calls are not available, and in all cases it provides quantification of the individual contributors to the ERF that are highly useful but not otherwise available.

Effects of square spatial periodic forcing on oscillatory hexagon patterns in coupled reaction-diffusion systems.

One of the central issues in pattern formation is understanding the response of pattern-forming systems to an external stimulus. While significant progress has been made in systems with only one instability, much less is known about the response of complex patterns arising from the interaction of two or more instabilities. In this paper, we consider the effects of square spatial periodic forcing on oscillatory hexagon patterns in a two-layer coupled reaction diffusion system which undergoes both Turing and Hopf instabilities. Two different types of additive forcings, namely direct and indirect forcing, have been applied. It is shown that the coupled system exhibits different responses towards the spatial forcing under different forcing types. In the indirect case, the oscillatory hexagon pattern transitions into other oscillatory Turing patterns or resonant Turing patterns, depending on the forcing wavenumber and strength. In the direct forcing case, only non-resonant Turing patterns can be obtained. Our results may provide new insight into the modification and control of spatio-temporal patterns in multilayered systems, especially in biological and ecological systems.

Development and Evaluation of E3SM‐MOSAIC: Spatial Distributions and Radiative Effects of Nitrate Aerosol

AbstractNitrate aerosol plays an important role in affecting regional air quality as well as Earth's climate. However, it is not well represented or even neglected in many global climate models. In this study, we couple the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) module with the four‐mode version of the Modal Aerosol Module (MAM4) in DOE's Energy Exascale Earth System Model version 2 (E3SMv2) to simulate nitrate aerosol and its radiative effects. We find that nitrate aerosol simulated by E3SMv2‐MAM4‐MOSAIC is sensitive to the treatment of gaseous HNO3 transfer to/from interstitial particles related to accommodation coefficients of HNO3 () on dust and non‐dust particles. We compare three different treatments of HNO3 transfer: (a) a treatment (MTC_SLOW) that uses a low in the mass transfer coefficient (MTC) calculation; (b) a dust‐weighted MTC treatment (MTC_WGT) that uses a high on non‐dust particles; and (c) a dust‐weighted MTC treatment that also splits coarse mode aerosols into the coarse dust and sea salt sub‐modes in MOSAIC (MTC_SPLC). MTC_WGT and MTC_SPLC increase the global annual mean (2005–2014) nitrate burden from 0.096 (MTC_SLOW) to 0.237 and 0.185 Tg N, respectively, mostly in the coarse mode. MTC_WGT and MTC_SPLC also produce stronger nitrate direct radiative forcing (−0.048 and −0.051 W m−2, respectively) and indirect forcing (−0.33 and −0.35 W m−2, respectively) than MTC_SLOW (−0.021 and −0.24 W m−2). MTC_WGT and MTC_SPLC improve nitrate surface concentrations over remote oceans based on limited observations and vertical profiles of nitrate concentrations against aircraft measurements below 400 hPa.

Impact of present and future aircraft NOxand aerosol emissions on atmospheric composition and associated direct radiative forcing of climate

Abstract. Aviation NOx emissions not only have an impact on global climate by changing ozone and methane levels but also contribute to the deterioration of local air quality. A new version of the LMDZ-INCA global model, including chemistry of both the troposphere and the stratosphere and the sulfate-nitrate-ammonium cycle, is applied to re-evaluate the impact of aircraft NOx and aerosol emissions on climate. The results confirm that the efficiency of NOx to produce ozone is very much dependent on the injection height; it increases with the background methane and NOx concentrations and with decreasing aircraft NOx emissions. The methane lifetime variation is less sensitive to the location of aircraft NOx emissions than the ozone change. The net NOx radiative forcing (RF) (O3+CH4) is largely affected by the revised CH4 RF formula. The ozone positive forcing and the methane negative forcing largely offset each other, resulting in a slightly positive forcing for the present day. However, in the future, the net forcing turns to negative, essentially due to higher methane background concentrations. Additional RFs involving particle formation arise from aircraft NOx emissions since the increased hydroxyl radical (OH) concentrations are responsible for an enhanced conversion of SO2 to sulfate particles. Aircraft NOx emissions also increase the formation of nitrate particles in the lower troposphere. However, in the upper troposphere, increased sulfate concentrations favour the titration of ammonia leading to lower ammonium nitrate concentrations. The climate forcing of aircraft NOx emissions is likely to be small or even switch to negative (cooling), depending on atmospheric NOx or CH4 future background concentrations, or when the NOx impact on sulfate and nitrate particles is considered. However, large uncertainties remain for the NOx net impact on climate and in particular on the indirect forcings associated with aerosols, which are even more uncertain than the other forcings from gaseous species. Hence, additional studies with a range of models are needed to provide a more consolidated view. Nevertheless, our results suggest that reducing aircraft NOx emissions is primarily beneficial for improving air quality.

Use of machine learning to reduce uncertainties in particle number concentration and aerosol indirect radiative forcing predicted by climate models

Use of machine learning to reduce uncertainties in particle number concentration and aerosol indirect radiative forcing predicted by climate models

Simulating the radiative forcing of oceanic dimethylsulfide (DMS) in Asia based on machine learning estimates

Abstract. Dimethylsulfide (DMS) emitted from seawater is a key precursor to new particle formation and acts as a regulator in Earth's warming climate system. However, DMS's effects are not well understood in various ocean regions. In this study, we estimated DMS emissions based on a machine learning method and used the GEOS-Chem global 3D chemical transport model coupled with the TwO Moment Aerosol Sectional (TOMAS) microphysics scheme to simulate the atmospheric chemistry and radiative effects of DMS. The contributions of DMS to atmospheric SO42- aerosol and cloud condensation nuclei (CCN) concentrations along with the radiative effects over the Asian region were evaluated for the first time. First, we constructed novel monthly resolved DMS emissions (0.5∘×0.5∘) for the year 2017 using a machine learning model; 4351 seawater DMS measurements (including the recent measurements made over the Chinese seas) and 12 relevant environment parameters were selected for model training. We found that the model could predict the observed DMS concentrations with a correlation coefficient of 0.75 and fill the values in regions lacking observations. Across the Asian seas, the highest seasonal mean DMS concentration occurred in March–April–May (MAM), and we estimate the annual DMS emission flux of 1.25 Tg (S), which is equivalent to 15.4 % of anthropogenic sulfur emissions over the entire simulation domain (which covered most of Asia) in 2017. The model estimates of DMS and methane sulfonic acid (MSA), using updated DMS emissions, were evaluated by comparing them with cruise survey experiments and long-term online measurement site data. The improvement in model performance can be observed compared with simulation results derived from the global-database DMS emissions. The relative contributions of DMS to SO42- and CCN were higher in remote oceanic areas, contributing 88 % and 42 % of all sources, respectively. Correspondingly, the sulfate direct radiative forcing (DRF) and indirect radiative forcing (IRF) contributed by DMS ranged from −200 to −20 mW m−2 and from −900 to −100 mW m−2, respectively, with levels varying by season. The strong negative IRF is mainly over remote ocean regions (−900 to −600 mW m−2). Generally, the magnitude of IRF derived by DMS was twice as large as its DRF. This work provides insights into the source strength of DMS and the impact of DMS on climate and addresses knowledge gaps related to factors controlling aerosols in the marine boundary layer and their climate impacts.

Multivariable statistical analysis between geomagnetic field, climate, and orbital periodicities over the last 500 KYR, and their relationships during the last interglacial

Relationships between geomagnetic field (GF) variations, paleoclimates, and Milankovitch cycles have increasingly attracted the attention of researchers mainly because of the assumption that GF may have acted as a climate forcing, suggesting that GF variations and orbital forcing may be linked in a complex synergistic way, especially, during interglacials and interstadials. We first performed an exhaustive analysis of the relationship between GF, a paleotemperature proxy, astroclimatic parameters, and the summer solstice mean daily insolation at 65 N over the last 500 kyr. We evaluated the relationship between the variables at the orbital scale, using wavelets, cross wavelets, and multiple cross wavelets. Our novel approach to the subject is the use of a new multiple cross wavelet algorithm, which allowed us to simultaneously analyze several data series and determine the relative phases between the signals. We confirm that the eccentricity modulates the GF behavior, and that the precession could have been related to some short-term GF variations. Both orbital parameters seem to be precursors of GF changes. Also, it is especially interesting to investigate the role of the GF reversion events because they could have acted as an indirect climate forcing, and we focused on the relationship among forcings during Marine Isotope Stage (MIS) 5. During this period, two GF reversions (Blake and post-Blake) could have been associated with relative climate cooling. The consequent lack or weakening of shielding associated with GF events and downward insolation, both influenced by orbital forcing, could finally have promoted a relative global climate cooling during MIS 5. • New multiple cross wavelets of RPI, δ 18 O, insolation, and orbital forcing. • GF is modulated by eccentricity in the trend, by precession in short-term changes. • Orbital forcing seems to be precursor of GF variations over the last 500 kyr. • Cooling is promoted by lows RPI and insolation, both influenced by orbital forcing.

Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing

Abstract. Aerosol indirect radiative forcing (IRF), which characterizes how aerosols alter cloud formation and properties, is very sensitive to the preindustrial (PI) aerosol burden. Dimethyl sulfide (DMS), emitted from the ocean, is a dominant natural precursor of non-sea-salt sulfate in the PI and pristine present-day (PD) atmospheres. Here we revisit the atmospheric oxidation chemistry of DMS, particularly under pristine conditions, and its impact on aerosol IRF. Based on previous laboratory studies, we expand the simplified DMS oxidation scheme used in the Community Atmospheric Model version 6 with chemistry (CAM6-chem) to capture the OH-addition pathway and the H-abstraction pathway and the associated isomerization branch. These additional oxidation channels of DMS produce several stable intermediate compounds, e.g., methanesulfonic acid (MSA) and hydroperoxymethyl thioformate (HPMTF), delay the formation of sulfate, and, hence, alter the spatial distribution of sulfate aerosol and radiative impacts. The expanded scheme improves the agreement between modeled and observed concentrations of DMS, MSA, HPMTF, and sulfate over most marine regions, based on the NASA Atmospheric Tomography (ATom), the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA), and the Variability of the American Monsoon Systems (VAMOS) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) measurements. We find that the global HPMTF burden and the burden of sulfate produced from DMS oxidation are relatively insensitive to the assumed isomerization rate, but the burden of HPMTF is very sensitive to a potential additional cloud loss. We find that global sulfate burden under PI and PD emissions increase to 412 Gg S (+29 %) and 582 Gg S (+8.8 %), respectively, compared to the standard simplified DMS oxidation scheme. The resulting annual mean global PD direct radiative effect of DMS-derived sulfate alone is −0.11 W m−2. The enhanced PI sulfate produced via the gas-phase chemistry updates alone dampens the aerosol IRF as anticipated (−2.2 W m−2 in standard versus −1.7 W m−2, with updated gas-phase chemistry). However, high clouds in the tropics and low clouds in the Southern Ocean appear particularly sensitive to the additional aqueous-phase pathways, counteracting this change (−2.3 W m−2). This study confirms the sensitivity of aerosol IRF to the PI aerosol loading and the need to better understand the processes controlling aerosol formation in the PI atmosphere and the cloud response to these changes.

An Optical Flow Approach to Tracking Ship Track Behavior Using GOES-R Satellite Imagery

Ship emissions can form linear cloud structures, or <italic xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">ship tracks</i> , when atmospheric water vapor condenses on aerosols in the ship exhaust. These structures are of interest because they are observable and traceable examples of MCB, a mechanism that has been studied as a potential approach for solar climate intervention. Ship tracks can be observed throughout the diurnal cycle via space-borne assets like the advanced baseline imagers on the national oceanic and atmospheric administration geostationary operational environmental satellites, the GOES-R series. Due to complex atmospheric dynamics, it can be difficult to track these aerosol perturbations over space and time to precisely characterize how long a single emission source can significantly contribute to indirect radiative forcing. We propose an optical flow approach to estimate the trajectories of ship-emitted aerosols after they begin mixing with low boundary layer clouds using GOES-17 satellite imagery. Most optical flow estimation methods have only been used to estimate large scale atmospheric motion. We demonstrate the ability of our approach to precisely isolate the movement of ship tracks in low-lying clouds from the movement of large swaths of high clouds that often dominate the scene. This efficient approach shows that ship tracks persist as visible, linear features beyond 9 h and sometimes longer than 24 h.

Slow-down in summer warming over Greenland in the past decade linked to central Pacific El Ni\xf1o

Greenland warming and ice loss have slowed down since the early 2010s, in contrast to the rest of the Arctic region. Both natural variability and anthropogenic forcing contribute to recent Greenland warming by reducing cloud cover and surface albedo, yet most climate models are unable to reasonably simulate the unforced natural variability. Here we show that a simplified atmospheric circulation model successfully simulates an atmospheric teleconnection from the tropics towards Greenland, which accounts for Greenland cooling through an intensified cyclonic circulation. Synthesis from observational analysis and model experiments indicate that over the last decade, more central Pacific El Niño events than canonical El Niño events have generated the atmospheric teleconnection by shifting the tropical rainfall zone poleward, which led to an intensified cyclonic circulation over Greenland. The intensified cyclonic circulation further extends into the Arctic Ocean in observations, whereas the model does not show a direct remote forcing from the tropics, implying the contribution of an indirect atmospheric forcing. We conclude that the frequent occurrence of central Pacific El Niño events has played a key role in the slow-down of Greenland warming and possibly Arctic sea-ice loss.

Secondary Inorganic Ions Characteristics in PM2.5 Along Offshore and Coastal Areas of the Megacity Shanghai

AbstractSecondary inorganic ions are important constituents of PM2.5 that play an important role in global climate change through direct and indirect radiative forcing. To investigate the influence of ship emissions on coastal cities, we launched a cruise ship campaign offshore of the East China Sea (ECS) and two field observation sites in the megacity of Shanghai using 1‐hr time‐resolved water‐soluble ion chromatography from June 3 to June 27, 2017. Three main secondary inorganic soluble ions in the atmosphere of the ECS, that is, non‐sea‐salt sulfate (nss‐SO42−), NO3− and NH4+, were 8.87, 4.94, and 4.65 μg m−3, respectively. While their values at the Pudong (PD) station in urban Shanghai were 6.33, 9.47, and 4.74 μg m−3 and at the Dianshanhu (DSH) station in suburban Shanghai were 7.33, 10.01, and 6.78 μg m−3, respectively. Nss‐SO42− was dominant in the PM2.5 in the atmosphere of the ECS (nss‐SO42−/NO3− = 1.8), and mainly distributed near the Zhoushan Islands of the ECS. This indicated significant contributions from ship emissions. Based on the Community Multiscale Air Quality model, two main sources of nss‐SO42− were identified: emissions and horizontal transport. These comprised over 90% of the nss‐SO42−. The influence of ship emissions reached up to 31.6% of the total nss‐SO42− alongside the cruise ship and near coastal parking ports in the Yangtze River Delta area, suggesting that more attention should be paid to ship emissions.

An airborne study of the aerosol effect on the dispersion of cloud droplets in a drizzling marine stratocumulus cloud over eastern China

Detailed airborne measurements were carried out to explore aerosol-cloud interactions and cloud microphysical properties in a drizzling marine stratocumulus cloud deck over eastern China. Results show that the collision-coalescence of cloud droplets, the condensation of small droplets, and the collision-induced break-up of drizzle were the dominant microphysical processes in the sampled water cloud parcel. The region in the vicinity of the cloud's lateral boundary was spatially divided into sub-regions to better understand aerosol and droplet interactions. Relationships between the relative dispersion (ε) and the cloud’'s microphysical and dynamical characteristics were also examined. A negative relation was found between ε and the cloud droplet number concentration, with ε showing a close relationship with the liquid water content (LWC) and updraft velocity. When LWC was greater than ~0.75 g kg−1, the range of ε values narrowed, and updrafts dominated. By introducing ε in the cloud droplet effect radius (Re) parameterization, we find that ε can further affect indirect forcing by changing the Re distribution for the cloud examined in this study. The dispersion effect (DE) was estimated using the effective radius ratio and the specific cloud water content. An in-depth analysis indicates that DE may offset the Twomey effect by ~12%. Two different methods of estimating the indirect effect (IE) yielded close values (0.084 and 0.077), suggesting that introducing DE into the estimation had a small influence on the IE calculation in the drizzling marine stratocumulus cloud of this study. Note that the estimated IE has a large uncertainty, given the large biases in the cloud properties measured.

Retrieval and Calculation of Vertical Aerosol Mass Fluxes by a Coherent Doppler Lidar and a Sun Photometer

The direct and indirect radiation forcing of aerosol particles deeply affect the energy budget and the atmospheric chemical and physical processes. To retrieve the vertical aerosol mass fluxes and to investigate the vertical transport process of aerosol by a coherent Doppler lidar (CDL), a practical method for instrumental calibration and aerosol optical properties retrieval based on CDL and sun photometer synchronization observations has been developed. A conversion of aerosol optical properties to aerosol microphysical properties is achieved by applying a well-developed algorithm. Furthermore, combining the vertical velocity measured simultaneously with a CDL, we use the eddy covariance (EC) method to retrieve the vertical turbulent aerosol mass fluxes by a CDL and sun photometer with a spatial resolution of 15 m and a temporal resolution of 1 s throughout the planetary boundary layer (PBL). In this paper, we present a measurement case of 24-h continuous fluxes observations and analyze the diurnal variation of the vertical velocity, the aerosol backscatter coefficient at 1550 nm, the mean aerosol mass concentration, and the vertical aerosol mass fluxes on 13 April 2020. Finally, the main relative errors in aerosol mass flux retrieval, including sample error σF,S, aerosol optical properties retrieval error σF,R, and error introduced from aerosol microphysical properties retrieval algorithm σF,I, are evaluated. The sample error σF,S is the dominating error which increases with height except during 12:00–13:12 LST. The aerosol optical properties retrieval error σF,R is 21% and the error introduced from the aerosol microphysical properties retrieval algorithm σF,I is less than 50%.

Constructing Shapes and Mixing Structures of Black Carbon Particles With Applications to Optical Calculations

AbstractBlack carbon (BC) aerosols strongly absorb the solar radiation, affecting the regional and global climate through direct and indirect radiative forcing. The optical properties of BC are critical factors to estimate their radiative forcing. However, the optical absorption of BC is still under controversy partially due to the weakness in quantifying their complex morphology and mixing structures. Although a Discrete Dipole Approximation (DDA) can calculate optical properties of fine particles with arbitrary shapes, an appropriate definition of realistic BC shape models for optical simulation is essentially required. Here we present a novel Electron‐Microscope‐to‐BC‐Simulation (EMBS) tool to construct realistic BC shape models with various morphology and mixing structures for optical calculation using DDA. The optical properties of BC particles with different particle morphology, coating thickness, and embedded fraction (F) are estimated based on electron microscope. We find that absorption enhancement (Eabs) of the realistic irregular model is larger than that of the present commonly used spherical model (i.e., BC aggregate with spherical coating). The BC core morphology greatly influences Eabs of the embedded BC particles with irregular coating when the volume‐equivalent‐diameter ratio of particle to core (Dp/Dc) is larger than 1.8. The F significantly influences Eabs of BC particles, suggesting that the mixing structure between coating and core is an important factor to determine the optical absorption of aged BC particles. The study highlights that the BC core morphology, coating shape, coating thickness, and mixing structures influence their optical properties and should be considered as important variables in climate models.