Abstract. The interactions between aerosols and ice clouds represent one of the largest uncertainties in global radiative forcing from pre-industrial time to the present. In particular, the impact of aerosols on ice crystal effective radius (Rei), which is a key parameter determining ice clouds' net radiative effect, is highly uncertain due to limited and conflicting observational evidence. Here we investigate the effects of aerosols on Rei under different meteorological conditions using 9-year satellite observations. We find that the responses of Rei to aerosol loadings are modulated by water vapor amount in conjunction with several other meteorological parameters. While there is a significant negative correlation between Rei and aerosol loading in moist conditions, consistent with the "Twomey effect" for liquid clouds, a strong positive correlation between the two occurs in dry conditions. Simulations based on a cloud parcel model suggest that water vapor modulates the relative importance of different ice nucleation modes, leading to the opposite aerosol impacts between moist and dry conditions. When ice clouds are decomposed into those generated from deep convection and formed in situ, the water vapor modulation remains in effect for both ice cloud types, although the sensitivities of Rei to aerosols differ noticeably between them due to distinct formation mechanisms. The water vapor modulation can largely explain the difference in the responses of Rei to aerosol loadings in various seasons. A proper representation of the water vapor modulation is essential for an accurate estimate of aerosol–cloud radiative forcing produced by ice clouds.
Aerosols interact with radiation and clouds. Substantial progress made over the past 40 years in observing, understanding, and modeling these processes helped quantify the imbalance in the Earth's radiation budget caused by anthropogenic aerosols, called aerosol radiative forcing, but uncertainties remain large. This review provides a new range of aerosol radiative forcing over the industrial era based on multiple, traceable, and arguable lines of evidence, including modeling approaches, theoretical considerations, and observations. Improved understanding of aerosol absorption and the causes of trends in surface radiative fluxes constrain the forcing from aerosol‐radiation interactions. A robust theoretical foundation and convincing evidence constrain the forcing caused by aerosol‐driven increases in liquid cloud droplet number concentration. However, the influence of anthropogenic aerosols on cloud liquid water content and cloud fraction is less clear, and the influence on mixed‐phase and ice clouds remains poorly constrained. Observed changes in surface temperature and radiative fluxes provide additional constraints. These multiple lines of evidence lead to a 68% confidence interval for the total aerosol effective radiative forcing of ‐1.6 to ‐0.6 W m−2, or ‐2.0 to ‐0.4 W m−2with a 90% likelihood. Those intervals are of similar width to the last Intergovernmental Panel on Climate Change assessment but shifted toward more negative values. The uncertainty will narrow in the future by continuing to critically combine multiple lines of evidence, especially those addressing industrial‐era changes in aerosol sources and aerosol effects on liquid cloud amount and on ice clouds.
more » « less- NSF-PAR ID:
- 10457346
- Author(s) / Creator(s):
- ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more »
- Publisher / Repository:
- DOI PREFIX: 10.1029
- Date Published:
- Journal Name:
- Reviews of Geophysics
- Volume:
- 58
- Issue:
- 1
- ISSN:
- 8755-1209
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
more » « less
-
more » « less
Abstract We incorporate the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) module in the Community Earth System Model version 2 (CESM2) Community Atmosphere Model Version 6 with interactive chemistry (CAM6‐chem), and couple it with the four mode version of the Modal Aerosol Module (MAM4). The MOSAIC module is used to simulate the thermodynamics of the gas‐aerosol mass exchange, with a special focus on simulating nitrate aerosol. By comparing against ground and satellite observations, we found that the MOSAIC/MAM4 scheme performs reasonably well in simulating spatiotemporal distributions of aerosols, including nitrate aerosol. We conducted a series of model experiments with and without nitrate aerosols, and examined the radiative effect (RE) associated with nitrate aerosols in 1975, 2000, and 2010, and accessed the radiative forcing (RF) of nitrate aerosols between the present day and pre‐industrial periods. Comparing with the nitrate aerosol RE, we predicted relatively small RF of anthropogenic nitrate aerosol from aerosol‐radiation interactions (RFari: −0.014 W m−2) and large RF from aerosol‐cloud interactions (RFaci: −0.219 W m−2). Regional signatures of nitrate RE/RF are noticeable and important: for instance, very small changes in REariin Europe and USA, but 2.8–3 times increases in REariin India and China from 1975 to 2010, while REaci/RFaciin China is a warming effect due to the competing effect between sulfate and nitrate aerosols as cloud condensation nuclei.
-
more » « less
Abstract The influence of aerosol particles on cloud reflectivity remains one of the largest sources of uncertainty in our understanding of anthropogenic climate change. Commercial shipping constitutes a large and concentrated aerosol perturbation in a meteorological regime where clouds have a disproportionally large effect on climate. Yet, to date, studies have been unable to detect climatologically relevant cloud radiative effects from shipping, despite models indicating that the cloud response should produce a sizable negative radiative forcing (perturbation to Earth's energy balance). We attribute a significant increase in cloud reflectivity to enhanced cloud droplet number concentrations within a major shipping corridor in the southeast Atlantic. Prevailing winds constrain emissions around the corridor, which cuts through a climatically important region of expansive low cloud cover. We use universal kriging, a classic geostatistical method, to estimate what cloud properties would have been in the absence of shipping. In the morning, cloud brightening is consistent with changes in microphysics alone, whereas in the afternoon, increases in cloud brightness from microphysical changes are offset by decreases in the total amount of cloud water. We calculate an effective radiative forcing within the southeast Atlantic shipping corridor of approximately −2 W/m2. Several years of data are required to identify a clear signal.
Extrapolating our results globally, we calculate an effective radiative forcing due to aerosol‐cloud interactions in low clouds of −1.0 W/m2(95% confidence interval: −1.6 to −0.4 W/m2). The unique setup in the southeast Atlantic could be an ideal test for the representation of aerosol‐cloud interactions in climate models.
-
more » « less
Abstract Secondary organic aerosols (SOA) have been identified as a potential source of depositional ice nucleating particles and thus may have a radiative effect on cirrus clouds. This study develops a global model to examine the radiative effect of SOA on cirrus clouds using different treatments for the size distribution of SOA. The SOA from new particle formation by organics and their subsequent growth has a radiative effect of 0.35 ± 0.06 W m−2, while the radiative effect of SOA calculated by assuming a fixed size distribution is 0.31 ± 0.08 W m−2. This positive radiative effect on cirrus clouds opposes the negative effect of anthropogenic soot on cirrus clouds. In addition, the inclusion of SOA as an ice nucleating particle changes the background ice crystal number concentration, which impacts the calculation of radiative forcing from other aerosols. The radiative forcing of aircraft soot is estimated to be −0.11 ± 0.03 W m−2when including SOA formed from new particle formation by organics and growth. This is less negative than simulations that do not include ice nucleation from SOA. The change in SOA formed from organic nucleation from the preindustrial period to the present day causes a positive forcing of 0.02 ± 0.04 W m−2. It is important to use a size distribution based on the explicit formation mechanism for SOA to calculate their radiative effects. The simulation using an assumed fixed size distribution incorrectly results in a negative forcing of SOA between the present day and preindustrial atmospheres because it does not correctly calculate the change of SOA in the accumulation mode.
-
more » « less
The WRF-simulated changes in clouds and climate due to the increased anthropogenic aerosols for the summers of 2002–08 (vs the 1970s) over eastern China were used to offline calculate the radiative forcings associated with aerosol–radiation (AR) and aerosol–cloud–radiation (ACR) interactions, which subsequently facilitated the interpretation of surface temperature changes. During this period, the increases of aerosol optical depth (ΔAOD) averaged over eastern China range from 0.18 in 2004 to 0.26 in 2007 as compared to corresponding cases in the 1970s, and the multiyear means (standard deviations) of AR and ACR forcings at the surface are −6.7 (0.58) and −3.5 (0.63) W m−2, respectively, indicating the importance of cloud changes in affecting both the aerosol climate forcing and its interannual variation. The simulated mean surface cooling is 0.35°C, dominated by AR and ACR with a positive (cooling) feedback associated with changes in meteorology (~10%), and two negative (warming) feedbacks associated with decreases in latent (~70%) and sensible (~20%) heat fluxes. More detailed spatial characteristics were analyzed using ensemble simulations for the year 2008. Three regions—Jing-Jin-Ji (ΔAOD ~ 0.63), Sichuan basin (ΔAOD ~ 0.31), and middle Yangtze River valley (ΔAOD ~ 0.26)—at different climate regimes were selected to investigate the relative roles of AR and ACR. While the AR forcing is closely related to ΔAOD values, the ACR forcing presents different regional characteristics owing to cloud changes. In addition, the surface heat flux feedbacks are also different between regions. The study thus illustrates that ACR forcing is useful as a diagnostic parameter to unravel the complexity of climate change to aerosol forcing over eastern China.
